Abu Bakar, NA, Ali, S, Hisamuddin, SN, Supangat, A, Langford, SJ & Roslan, NA 2022, 'Effect of different deposition techniques of PCDTBT:PC71BM composite on the performance of capacitive-type humidity sensors', Synthetic Metals, vol. 285, pp. 117020-117020.
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Ali, S, Jameel, MA, Gupta, A, Shafiei, M & Langford, SJ 2022, 'A room temperature functioning ammonia sensor utilising a bis-phenylalanine naphthalene diimide', Sensors and Actuators A: Physical, vol. 348, pp. 114008-114008.
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Ali, S, Jameel, MA, Harrison, CJ, Gupta, A, Shafiei, M & Langford, SJ 2022, 'Nanoporous naphthalene diimide surface enhances humidity and ammonia sensing at room temperature', Sensors and Actuators B: Chemical, vol. 351, pp. 130972-130972.
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Angeloski, A, Price, JR, Ennis, C, Smith, K, McDonagh, AM, Dowd, A, Thomas, P, Cortie, M, Appadoo, D & Bhadbhade, M 2022, 'Thermosalience Revealed on the Atomic Scale: Rapid Synchrotron Techniques Uncover Molecular Motion Preceding Crystal Jumping', Crystal Growth & Design, vol. 22, no. 3, pp. 1951-1959.
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The solid-state phase transformation in nickel(II) bis(diisopropyldithiocarbonate) is analyzed using a combination of high-speed in situ single-crystal diffraction, terahertz spectroscopy, optical microscopy, thermal analysis, and density functional theory. We show that the monoclinic P21/c structure of this compound undergoes a displacive phase change at about 3 °C. The monoclinic angles and unit cell volumes change reversibly between 110.3°/2265 Å3 and 103.8°/2168 Å3. An analysis of atomic positions using high-resolution in situ synchrotron X-ray diffraction data revealed details of the atomic displacements that show a change in order that precedes and accompanies the change in structure. The structural changes are rapid and are manifested as reversible macroscale crystal movement and jumping (thermosalience) and represent the first case of thermosalience in dithiocarbamate complexes.
Bai, L, Song, A, Lei, X, Zhang, T, Song, S, Tian, H, Liu, H, Qin, X, Wang, G & Shao, G 2022, 'Hierarchical construction of hollow NiCo2S4 nanotube@NiCo2S4 nanosheet arrays on Ni foam as an efficient and durable electrocatalyst for hydrogen evolution reaction', International Journal of Hydrogen Energy, vol. 47, no. 91, pp. 38524-38532.
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Ternary transition metal chalcogenide (TTMC) with multicomponent, different phases and unique electronic structures have been studied in electrocatalytic hydrogen evolution reaction (HER). However, the strong interaction between adsorbed H (H∗) and sulfur leads to the unfavorable hydrogen desorption properties of considerable TTMC. Herein, we constructed the hierarchical hollow NiCo2S4 nanotube@NiCo2S4 nanosheet arrays on Ni foam substrate (NT-NiCo2S4@NS-NiCo2S4/NF) by ion-exchange method. Homogeneous anion diffusion facilitates the formation of regular ultrathin nanosheets on hollow NiCo2S4 nanotube arrays, which presents hierarchical architecture with more surface area and channels to active site exposure, electrolyte diffusion, and gas desorption for HER. As-synthesized optimal NT-NiCo2S4@NS-NiCo2S4/NF electrode demonstrates an excellent HER activity, especially an overpotential of 221 mV, a Tafel slope of 108 mV dec−1, and remarkable stability at current densities of 100 mA cm−2 in 1.0 M NaOH electrolyte.
Bake, A, Rahman, MR, Evans, PJ, Cortie, M, Nancarrow, M, Abrudan, R, Radu, F, Khaydukov, Y, Causer, G, Livesey, KL, Callori, S, Mitchell, DRG, Pastuovic, Z, Wang, X & Cortie, D 2022, 'Ultra-small cobalt particles embedded in titania by ion beam synthesis: Additional datasets including electron microscopy, neutron reflectometry, modelling outputs and particle size analysis', Data in Brief, vol. 40, pp. 107674-107674.
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Belay, Y, Muller, A & Williams, DBG 2022, 'Lanthanum-1,2,3-Triazole-Based 2D Coordination Polymer is an Efficient Catalyst for the Oxidation of Olefins', Inorganic Chemistry, vol. 61, no. 21, pp. 8226-8232.
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Cao, X, Huo, J, Li, L, Qu, J, Zhao, Y, Chen, W, Liu, C, Liu, H & Wang, G 2022, 'Recent Advances in Engineered Ru‐Based Electrocatalysts for the Hydrogen/Oxygen Conversion Reactions', Advanced Energy Materials, vol. 12, no. 41, pp. 2202119-2202119.
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AbstractThe application of renewable energy conversion devices is considered as one of the effective ways to alleviate the energy shortage and environmental pollution. Designing electrocatalysts with excellent performance and affordable price is promising to accelerate the reaction process and large‐scale application. At present, ruthenium (Ru)‐based nanomaterials have shown similar catalytic activity but superior price demand compared to commercial Pt/C. This undoubtedly makes Ru‐based nanomaterials a perfect candidate to replace advanced Pt catalysts. Significant progress is made in the rational design of Ru‐based electrocatalysts, but an in‐depth understanding of the engineering strategies and induced effects is still at an early stage. This review summarizes the modification strategies for enhancing the catalytic activity of Ru, including surface structure, metal element, nonmetal element, size, bimetallic oxides, and heterostructure engineering strategies. Then the induced electronic modulation effects generated by the intramolecular and intermolecular of the Ru‐based nanomaterials are elucidated. Further, the application progress of engineered Ru‐based nanomaterials for hydrogen and oxygen conversion reactions is highlighted, and the correlations of engineering strategies, catalytic activity, and reaction pathways are elaborated. Finally, challenges and prospects are presented for the future development and practical application of Ru‐based nanomaterials.
Che, S, Zhang, L, Wang, T, Su, D & Wang, C 2022, 'Graphitic Carbon Nitride‐Based Photocatalysts for Biological Applications', Advanced Sustainable Systems, vol. 6, no. 1, pp. 2100294-2100294.
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AbstractMetal‐free graphitic carbon nitride (g‐C3N4) as a newly emerging nanomaterial has been employed in the biomedical field because of its special optical and electrical characterizations. This review summarizes diverse methods for preparing g‐C3N4‐based materials, and discusses contemporary advancements in biosensors, photocatalytic sterilization, photodynamic therapy, drug carrier, and biological imaging. The biosafety and toxicity evaluations of g‐C3N4‐based materials are discussed as well. The review ends with an overview and several insights on the challenges and opportunities of g‐C3N4‐based nanomaterials in this burgeoning field. This review is expected to provide inspiration for developing future g‐C3N4‐based materials for the biomedical applications.
Che, S, Zhou, X, Zhang, L, Su, D, Wang, T & Wang, C 2022, 'Construction of a 2D Layered Phosphorus‐doped Graphitic Carbon Nitride/BiOBr Heterojunction for Highly Efficient Photocatalytic Disinfection', Chemistry – An Asian Journal, vol. 17, no. 11, p. e202200095.
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AbstractInfectious diseases caused by bacteria intimidate the health of human beings all over the world. Although many avenues have been tried, various operating conditions limit their actual applications. Photocatalytic nanomaterials are becoming candidates to be competent for water purification. Here, a novel and more efficient S‐scheme has been engineered between two dimensional (2D) layered phosphorus‐doped graphitic carbon nitride (P‐g‐C3N4) and BiOBr via hydrothermal polymerization to inhibit the recombination of charge and broaden light absorption. The as‐prepared P‐g‐C3N4/BiOBr hybrids exhibits significantly improved photocatalytic disinfection contrast to g‐C3N4/BiOBr in visible wavelengths, suggesting phosphorus doping which adjusts the band structure plays a significant role in the S‐scheme system. And the sterilization rate of multidrug‐resistant Acinetobacter baumannii 28 (AB 28) was 99.9999% within 80 min and Staphylococcus aureus (S. aureus) was 99.9%.
Chen, J, Xiao, J, Li, J, Gao, H, Guo, X, Liu, H & Wang, G 2022, 'Nano-engineering induced Bi dots in situ anchored into modified porous carbon with superior sodium ion storage', Journal of Materials Chemistry A, vol. 10, no. 38, pp. 20635-20645.
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As the anode of sodium ion batteries, Bi dots in situ embedded in a 3D porous carbon matrix (Bi@MC) enables high ICE (88.13%) and long cycle life with 100% capacity retention at 2.5 A g−1.
Chong, H, Fang, S, Yang, D, Tan, C, Wei, J, Chang, S-H, Fan, H, Yao, H, Qin, A, Shao, H, Zhang, Y, Leng, J, Su, D, Wang, C & Li, H 2022, 'Toxicity assessments and transcriptional effects of monofunctionalized Pt(II) complex under dark and light irradiation condition in Caenorhabditis elegans', Journal of Inorganic Biochemistry, vol. 230, pp. 111720-111720.
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In vivo toxicity of aromatic ring (BODIPY, 1,3,5,7,8-pentamethyl dipyrrin borondifluoride) attached monofunctional Pt(II) complexes mCBP {[cis-Pt(NH3)2Cl] 8-(para-pyridine-methylene),1,3,5,7-tetramethyl dipyrrin borondifluoride}+ Nitrate- and dCBP {[cis-Pt(NH3)2Cl]28-(1,3-pyrimidine-5-methylene),1,3,5,7-tetramethyl dipyrrin borondifluoride}2+ diNitrate2- were tested in Caenorhabditis elegans (C. elegans). dCBP showed promising reactive oxygen ROS (reactive oxygen species) generating capability. This complex resulted reduction of lifespan, body length and egg laying rate under dark and light irradiation in both N2 (wild-type, cisplatin resistant) and ok938 (asna-1, cisplatin sensitive) C. elegans. Expressional change of several key cancer related pathway (JNK (c-Jun N-terminal kinase) and Wnt/β-catenin (Wingless/Integrated/β-catenin)) related genes (for instance, jnk-1, wrm-1 and gst-4) were confirmed by RNA sequencing experiments. These transcriptional alternations could explain physiological parameters change in nematode and partially revealed how both Pt(II) based complexes influence cancer related pathways. Furthermore, these associated genes exhibited the function of apoptosis, reduced chemoresistance of cancer cells and most of those expressional changes were linked to extended survival of cancer patients.
Cui, L, Wang, Z, Kang, S, Fang, Y, Chen, Y, Gao, W, Zhang, Z, Gao, X, Song, C, Chen, X, Wang, Y & Wang, G 2022, 'N, P Codoped Hollow Carbon Nanospheres Decorated with MoSe2 Ultrathin Nanosheets for Efficient Potassium-Ion Storage', ACS Applied Materials & Interfaces, vol. 14, no. 10, pp. 12551-12561.
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Potassium-ion batteries (KIBs) are gradually being considered as an alternative for lithium-ion batteries because of their non-negligible advantages such as abundance and low expenditure of K, as well as higher electrochemical potential than another alternative─sodium-ion batteries. Nevertheless, when the electrode materials are inserted and extracted with large-sized K+ ions, the tremendous volume change will cause the collapse of the microstructures of electrodes and make the charging/discharging process irreversible, thus disapproving their extended application. In response to this, we put forward a feasible strategy to realize the in situ assembly of layered MoSe2 nanosheets onto N, P codoped hollow carbon nanospheres (MoSe2/NP-HCNSs) through thermal annealing and heteroatom doping strategies, and the resulting nanoengineered material can function well as an anode for KIBs. This cleverly designed nanostructure of MoSe2/NP-HCNS can broaden the interlayer spacing of MoSe2 to boost the efficiency of the insertion/extraction of K ions and also can accommodate large volume change-caused mechanical strain, facilitate electrolyte penetration, and prevent the aggregation of MoSe2 nanosheets. This synthetic method generates abundant defects to increase the amounts of active sites, as well as conductivity. The hierarchical nanostructure can effectively increase the proportion of pseudo-capacitance and promote interfacial electronic transfer and K+ diffusion, thus imparting great electrochemical performance. The MoSe2/NP-HCNS anode exhibits a high reversible capacity of 239.9 mA h g-1 at 0.1 A g-1 after 200 cycles and an ultralong cycling life of 161.1 mA h g-1 at 1 A g-1 for a long period of 1000 cycles. This nanoengineering method opens up new insights into the development of promising anode materials for KIBs.
Dai, Y, Zhang, X, Liu, Y, Yu, H, Su, W, Zhou, J, Ye, Q & Huang, Z 2022, '1,6;2,3-Bis-BN Cyclohexane: Synthesis, Structure, and Hydrogen Release', Journal of the American Chemical Society, vol. 144, no. 19, pp. 8434-8438.
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BN/CC isosterism has been widely investigated as a strategy to expand carbon-based compounds. The introduction of BN units in organic molecules always results in novel properties. In this work, we reported the first synthesis and characterization of 1,6;2,3-bis-BN cyclohexane, an isostere of cyclohexane with two adjacent BN pairs. Its ring flipping barrier is similar to that of cyclohexane. Protic hydrogens on N in 1,6;2,3-bis-BN cyclohexane show higher reactivity than its isomeric bis-BN cyclohexane. This compound exhibits an appealing hydrogen storage capability of >9.0 wt %, nearly twice as much as the 1,2;4,5-bis-BN cyclohexane.
Faisal, SN & Iacopi, F 2022, 'Thin-Film Electrodes Based on Two-Dimensional Nanomaterials for Neural Interfaces', ACS Applied Nano Materials, vol. 5, no. 8, pp. 10137-10150.
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Farahmandjou, M, Zhao, S, Lai, W-H, Sun, B, Notten, PHL & Wang, G 2022, 'Oxygen redox chemistry in lithium-rich cathode materials for Li-ion batteries: Understanding from atomic structure to nano-engineering', Nano Materials Science, vol. 4, no. 4, pp. 322-338.
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Gao, H, Tang, K, Xiao, J, Guo, X, Chen, W, Liu, H & Wang, G 2022, 'Recent advances in “water in salt” electrolytes for aqueous rechargeable monovalent-ion (Li+, Na+, K+) batteries', Journal of Energy Chemistry, vol. 69, pp. 84-99.
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Aqueous rechargeable batteries have attracted enormous attention owning to their intrinsic characteristics of non-flammability, low cost, and the superior ionic conductivity of the aqueous electrolyte. However, the narrow electrochemical stability window (1.23 V), imposed by hydrogen and oxygen evolution, constrains the overall energy density of batteries. The revolutionary “water-in-salt” electrolytes considerably expand the electrochemical stability window to 3 or even 4 volts, giving rise to a new series of high-voltage aqueous metal-ion chemistries. Herein, the recent advances in “water-in-salt” electrolytes for aqueous monovalent-ion (Li+, Na+, K+) rechargeable batteries have been systematically reviewed. Meanwhile, the corresponding reaction mechanisms, electrochemical performances and the existing challenges and opportunities are also highlighted.
Guo, X, Gao, H, Wang, S, Yang, G, Zhang, X, Zhang, J, Liu, H & Wang, G 2022, 'MXene-Based Aerogel Anchored with Antimony Single Atoms and Quantum Dots for High-Performance Potassium-Ion Batteries', Nano Letters, vol. 22, no. 3, pp. 1225-1232.
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Rationally electronic structure engineering of nanocomposite electrodes shows great promise for enhancing the electrochemical performance of rechargeable batteries. Herein, we report antimony single atoms and quantum dots (∼5 nm) codecorated Ti3C2Tx MXene-based aerogels (Sb SQ@MA) for high-performance potassium-ion batteries (PIBs). We found that the atomically dispersed Sb could modify the electronic structure of the Sb/Ti3C2Tx composite, improve the charge transfer kinetics, and enhance the potassium storage capability at the heterointerfaces. Additionally, the MXene-based aerogel with rich surface functional groups and defects provides abundant anchoring sites and endows the composite reinforced structural stability and highly efficient electron transfer. The high loading of Sb (∼60.3 wt %) with short ionic transport pathways is desired potassium reservoirs. These features synergistically enhance the rate and cycling performance of the Sb SQ@MA electrodes in PIBs. This work has demonstrated an enlightening technique to tailor the interface activity of heterostructured electrodes for electrochemical applications.
Guo, Z, Wang, T, Liu, H, Qiu, S, Zhang, X, Xu, Y, Langford, SJ & Sun, C 2022, 'Theoretical investigation of novel p-block metal-based electrocatalysts for nitrogen reduction reaction', Applied Surface Science, vol. 572, pp. 151441-151441.
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Han, C, Han, R, Zhang, X, Xu, Z, Li, W, Yamauchi, Y & Huang, Z 2022, '2D boron nanosheet architectonics: opening new territories by smart functionalization', Journal of Materials Chemistry A, vol. 10, no. 6, pp. 2736-2750.
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The lack of stability hinders the applications of pristine borophene. Functionalization imparts both stability and tunable properties allowing for wide application. This review focuses on the applications of functionalized 2D boron nanosheets.
Han, C, Li, W, Wang, J & Huang, Z 2022, 'Boron leaching: Creating vacancy-rich Ni for enhanced hydrogen evolution', Nano Research, vol. 15, no. 3, pp. 1868-1873.
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Creating vacancy is often highly effective in enhancing the hydrogen evolution performance of transition metal-based catalysts. Vacancy-rich Ni nanosheets have been fabricated via topochemical formation of two-dimentional (2D) Ni2B on graphene precursor followed by boron leaching. Anchored on graphene, a few atomic layered Ni2B nanosheets are first obtained by reduction and annealing. Large number of atomic vacancies are then generated in the Ni2B layer via leaching boron atoms. When used for hydrogen evolution reaction (HER), the vacancy-rich Ni/Ni(OH)2 heterostructure nanosheets demonstrate remarkable performance with a low overpotential of 159 mV at a current density of 10 mA·cm−2 in alkaline solution, a dramatic improvement over 262 mV of its precursor. This enhancement is associated with the formation of vacancies which introduce more active sites for HER along Ni/Ni(OH)2 heterointerfaces. This work offers a facile and universal route to introduce vacancies and improve catalytic activity. [Figure not available: see fulltext.]
Hou, J, Fang, L, Wang, X, Gao, H & Wang, G 2022, 'Spatially confined magnesiothermic reduction induced uniform mesoporous hollow silicon carbide nanospheres for high-performance supercapacitors', Chemical Communications, vol. 58, no. 89, pp. 12455-12458.
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Well-dispersed mesoporous hollow SiC nanospheres (∼95 nm in diameter) were fabricated via in situ magnesiothermic reduction. The unique construction enables a high-rate capacitance (τ0 of only 0.34 s) and long cycle stability for supercapacitors.
Hou, J, Yang, M, Sun, B & Wang, G 2022, 'Improvement Strategies toward Stable Lithium‐Metal Anodes for High‐Energy Batteries', Batteries & Supercaps, vol. 5, no. 12.
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AbstractLithium‐metal (Li‐metal) batteries are one of the most potential energy storage devices available these days. However, uncontrollable lithium dendritic growth and parasitic reactions lead to poor cycling efficiency and severe safety concerns, which restricts the use of Li‐metal batteries in practical applications. This article reviews the current development status of Li‐metal anodes, including investigations of reaction mechanisms and performance improvement strategies. In addition, future opportunities for developing safe and high‐performance Li‐metal batteries are also outlined.
Hou, W, Feng, P, Guo, X, Wang, Z, Bai, Z, Bai, Y, Wang, G & Sun, K 2022, 'Catalytic Mechanism of Oxygen Vacancies in Perovskite Oxides for Lithium–Sulfur Batteries', Advanced Materials, vol. 34, no. 26, pp. e2202222-2202222.
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AbstractDefective materials have been demonstrated to possess adsorptive and catalytic properties in lithium–sulfur (Li–S) batteries, which can effectively solve the problems of lithium polysulfides (LiPSs) shuttle and sluggish conversion kinetics during charging and discharging of Li–S batteries. However, there is still a lack of research on the quantitative relationship between the defect concentration and the adsorptive‐catalytic performance of the electrode. In this work, perovskites Sr0.9Ti1−xMnxO3−δ (STMnx) (x = 0.1–0.3) with different oxygen‐vacancy concentrations are quantitatively regulated as research models. Through a series of tests of the adsorptive property and electrochemical performance, a quantitative relationship between oxygen‐vacancy concentration and adsorptive‐catalytic properties is established. Furthermore, the catalytic mechanism of oxygen vacancies in Li–S batteries is investigated using density functional theory calculations and in situ experiments. The increased oxygen vacancies can effectively increase the binding energy between perovskite and LiPSs, reduce the energy barrier of LiPSs decomposition reaction, and promote LiPSs conversion reaction kinetics. Therefore, the perovskite STMn0.3 with high oxygen‐vacancy concentrations exhibits excellent LiPSs adsorptive and catalytic properties, realizing high‐efficiency Li–S batteries. This work is helpful to realize the application of the quantitative regulation strategy of defect engineering in Li–S batteries.
Iacopi, F & Lin, C-T 2022, 'A perspective on electroencephalography sensors for brain-computer interfaces', Progress in Biomedical Engineering, vol. 4, no. 4, pp. 043002-043002.
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Abstract This Perspective offers a concise overview of the current, state-of-the-art, neural sensors for brain-machine interfaces, with particular attention towards brain-controlled robotics. We first describe current approaches, decoding models and associated choice of common paradigms, and their relation to the position and requirements of the neural sensors. While implanted intracortical sensors offer unparalleled spatial, temporal and frequency resolution, the risks related to surgery and post-surgery complications pose a significant barrier to deployment beyond severely disabled individuals. For less critical and larger scale applications, we emphasize the need to further develop dry scalp electroencephalography (EEG) sensors as non-invasive probes with high sensitivity, accuracy, comfort and robustness for prolonged and repeated use. In particular, as many of the employed paradigms require placing EEG sensors in hairy areas of the scalp, ensuring the aforementioned requirements becomes particularly challenging. Nevertheless, neural sensing technologies in this area are accelerating thanks to the advancement of miniaturised technologies and the engineering of novel biocompatible nanomaterials. The development of novel multifunctional nanomaterials is also expected to enable the integration of redundancy by probing the same type of information through different mechanisms for increased accuracy, as well as the integration of complementary and synergetic functions that could range from the monitoring of physiological states to incorporating optical imaging.
Ibrahim, I, Hossain, SM, Seo, DH, McDonagh, A, Foster, T, Shon, HK & Tijing, L 2022, 'Insight into the role of polydopamine nanostructures on nickel foam-based photothermal materials for solar water evaporation', Separation and Purification Technology, vol. 293, pp. 121054-121054.
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Ibrahim, I, Seo, DH, Park, MJ, Angeloski, A, McDonagh, A, Bendavid, A, Shon, HK & Tijing, L 2022, 'Highly stable gold nanolayer membrane for efficient solar water evaporation under a harsh environment', Chemosphere, vol. 299, pp. 134394-134394.
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Ibrar, I, Yadav, S, Altaee, A, Safaei, J, Samal, AK, Subbiah, S, Millar, G, Deka, P & Zhou, J 2022, 'Sodium docusate as a cleaning agent for forward osmosis membranes fouled by landfill leachate wastewater', Chemosphere, vol. 308, no. Pt 2, pp. 136237-136237.
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Membrane cleaning is critical for economic and scientific reasons in wastewater treatment systems. Sodium docusate is a laxative agent and removes cerumen (ear wax). Docusate penetrates the hard ear wax, making it softer and easier to remove. The same concept could be applied to soften and remove fouling layers on the membrane surface. Once softened, the foulants can be easily flushed with water. This innovative approach can address the challenge of developing superior methods to mitigate membrane fouling and material degradation. In this study, we evaluated the efficiency of sodium docusate for cleaning fouled forward osmosis membranes with real landfill leachate wastewater. Experiments were conducted to examine the impact of dose rate, contact time, flow or static conditions, and process configuration (forward osmosis (FO) or pressure retarded osmosis (PRO) upon fouling created by landfill leachate dewatering. A remarkable (99%) flux recovery was achieved using docusate at a small concentration of only 0.1% for 30 min. Furthermore, docusate can also effectively restore flux with static cleaning without using pumps to circulate the cleaning solution. Furthermore, cleaning efficiency can be achieved at neutral pH compatible with most membrane materials. From an economic and energy-saving perspective, static cleaning can almost achieve the same cleaning efficiency as kinetic cleaning for fouled forward osmosis membranes without the expense of additional pumping energy compared to kinetic cleaning. Since pumping energy is a major contributor to the overall energy of the forward osmosis system, it can be minimized to a certain degree by using a static cleaning approach and can bring good energy savings when using larger membrane areas. Studies of the contact angle on the membrane surface indicated that the contact angle was decreased compared to the fouled membrane after cleaning (e.g. 70.3° to 63.2° or FO mode and static cleaning). Scanning Electron Micro...
Irvine, CP, Stopic, A, Westerhausen, MT, Phillips, MR & Ton-That, C 2022, 'Enhancement of excitonic and defect-related luminescence in neutron transmutation doped β−Ga2O3', Physical Review Materials, vol. 6, no. 11, p. 114603.
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Neutron irradiation analysis, inductively coupled plasma mass spectrometry (ICPMS), and cathodoluminescence (CL) spectroscopy are used to investigate the influence of transmuted Ge incorporation on the luminescence properties of β-Ga2O3 single crystals. Calculations based on Ga2O3-neutron interaction reveal temporal variations of both Ge and Zn concentrations as a function of time during and after neutron irradiation. To produce a concentration of 5×1018Gedonors/cm3 from the neutron transmutation of Ga, the β-Ga2O3 crystal was irradiated for 27 h, which was accompanied by the incorporation of 1016Znacceptors/cm3. These calculated dopant concentrations are confirmed by ICPMS. The β-Ga2O3 crystals exhibit a UV band at 3.40 eV due to self-trapped holes (STHs) and two blue donor-acceptor pair (DAP) peaks at 3.14 eV (BL1) and 2.92 eV (BL2). In addition to the neutron-induced incorporation of substitutional Ge donors and Zn acceptors on Ga sites, Ga vacancies (VGa) were created by high-energy neutrons in the flux, which strongly enhanced the BL1 peak. The VGa acceptors compensate the neutron-induced Ge donors, making the Ga2O3 crystal highly resistive. Concurrent temperature-resolved CL measurements of the β-Ga2O3 before and after neutron irradiation reveal a twofold increase in both the STH and BL1 peaks. This result suggests that STHs are preferentially localized at an O site adjacent to VGa, as theoretically predicted by Kananen et al. [Appl. Phys. Lett. 110, 202104 (2017)10.1063/1.4983814.]. Analysis of the Ga2O3 CL temperature dependence reveals that the UV and BL1 bands after the neutron irradiation exhibit an equivalent activation energy of 100±10meV due to the presence of a neutron-induced defect that acts as an efficient competitive nonradiative recombination channel. The results also provide evidence that the BL1 and BL2 bands arise from different DAP pairs.
Jiang, S, Suo, H, Zheng, X, Zhang, T, Lei, Y, Wang, Y, Lai, W & Wang, G 2022, 'Lightest Metal Leads to Big Change: Lithium‐Mediated Metal Oxides for Oxygen Evolution Reaction', Advanced Energy Materials, vol. 12, no. 33, pp. 2201934-2201934.
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AbstractAs the lightest metal, the reversible insertion/extraction properties of lithium have been key findings in lithium metal oxide chemistry. Lithium has been widely used in the oxygen evolution reaction (OER), and the reaction mechanism of lithium‐mediated metal oxides has both similarities and uniqueness compared to typical dual metal oxides. Notably, the insertion/extraction of lithium during the OER is also crucial for the construction of novel surface reconstruction models. This review aims to provide the concepts of general OER pathways and key features of dual metal oxides for the OER. As a comparison then the development of lithium metal oxides for the OER is introduced and the chemistry underlying lithium metal oxide catalysts is unveiled. This review also examines the challenges remaining for the relevant catalysts, with prospects for further improving their OER activities.
Ju, Z, Zhao, Q, Chao, D, Hou, Y, Pan, H, Sun, W, Yuan, Z, Li, H, Ma, T, Su, D & Jia, B 2022, 'Energetic Aqueous Batteries', Advanced Energy Materials, vol. 12, no. 27, pp. 2201074-2201074.
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AbstractRechargeable aqueous batteries are considered to be one of the most effective energy storage technologies to balance the cost‐efficiency, safety, and energy/power demands. The further progress of aqueous batteries with high energy density is needed to meet the ever‐increasing energy‐storage demands. This review highlights the strategies proposed so far to pursue the high energy density aqueous batteries, including the aspects of the electrolytes (from concentrated to dilute), the electrode chemistry (from inserted to converted), the cathode materials (from inorganic to organic), the anode materials (from compound to metallic), and the battery configurations (from integrated to decoupled). Critical appraisals of the emerging electrochemistry are presented for addressing the key issues in boosting the energy densities. Finally, the authors render insights into the future development of high‐energy aqueous batteries.
Katzmarek, DA, Pradeepkumar, A, Ziolkowski, RW & Iacopi, F 2022, 'Review of graphene for the generation, manipulation, and detection of electromagnetic fields from microwave to terahertz', 2D Materials, vol. 9, no. 2, pp. 022002-022002.
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AbstractGraphene has attracted considerable attention ever since the discovery of its unprecedented properties, including its extraordinary and tunable electronic and optical properties. In particular, applications within the microwave to terahertz frequency spectrum can benefit from graphene’s high electrical conductivity, mechanical flexibility and robustness, transparency, support of surface-plasmon-polaritons, and the possibility of dynamic tunability with direct current to light sources. This review aims to provide an in-depth analysis of current trends, challenges, and prospects within the research areas of generating, manipulating, and detecting electromagnetic fields using graphene-based devices that operate from microwave to terahertz frequencies. The properties of and models describing graphene are reviewed first, notably those of importance to electromagnetic applications. State-of-the-art graphene-based antennas, such as resonant and leaky-wave antennas, are discussed next. A critical evaluation of the performance and limitations within each particular technology is given. Graphene-based metasurfaces and devices used to manipulate electromagnetic fields, e.g. wavefront engineering, are then examined. Lastly, the state-of-the-art of detecting electromagnetic fields using graphene-based devices is discussed.
Khan, K, Tareen, AK, Iqbal, M, Zhang, Y, Mahmood, A, Mahmood, N, Yin, J, Khatoon, R & Zhang, H 2022, 'Recent advance in MXenes: New horizons in electrocatalysis and environmental remediation technologies', Progress in Solid State Chemistry, vol. 68, pp. 100370-100370.
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Khodasevych, I, Rufangura, P & Iacopi, F 2022, 'Designing concentric nanoparticles for surface-enhanced light-matter interaction in the mid-infrared', Optics Express, vol. 30, no. 13, pp. 24118-24118.
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Nanosized particles with high responsivity in the infrared spectrum are of great interest for biomedical applications. We derive a closed-form expression for the polarizability of nanoparticles made of up to three concentric nanolayers consisting of a frequency dependent polar dielectric core, low permittivity dielectric spacer shell and conductive graphene outer shell, using the electrostatic Mie theory in combination with conductive layer in a dipole approximation. We use the obtained formula to investigate SiC, GaN and hBN as core materials, and graphene as conductive shell, separated by a low-permittivity dielectric spacer. Three-layer nanoparticles demonstrate up to a 12-fold increased mid-infrared (MIR) absorption as compared to their monolithic polar dielectrics, and up to 1.7 as compared to two-layer (no spacer) counterparts. They also show orders of magnitude enhancement of the nanoparticle scattering efficiency. The enhancement originates from the phonon-plasmon hybridization thanks to the graphene and polar dielectric combination, assisted by coupling via the low permittivity spacer, resulting in the splitting of the dielectric resonance into two modes. Those modes extend beyond the dielectric’s Reststrahlen band and can be tuned by tailoring the nanoparticles characteristics as they can be easily calculated through the closed-form expression. Nanoparticles with dual band resonances and enhanced absorption and scattering efficiencies in the MIR are of high technological interest for biomedical applications, such as surface -enhanced vibrational spectroscopies allowing simultaneous imaging and spectroscopy of samples, as well as assisting guided drug delivery.
Kumar, S, Lyalin, A, Huang, Z & Taketsugu, T 2022, 'Catalytic Oxidative Dehydrogenation of Light Alkanes over Oxygen Functionalized Hexagonal Boron Nitride', ChemistrySelect, vol. 7, no. 1.
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AbstractThe catalytic activity of oxygen functionalized hexagonal boron nitride (h‐BN) with >B−O−O−B< and >B−O−B< active sites at the zigzag edges for oxidative dehydrogenation (ODH) of light alkanes, specifically ethane (C2H6), propane (C3H8), butane (C4H10), and isobutane (HC(CH3)3) is explored. It has been found that the reaction pathway involves two H atom transfer steps with small activation energies. We demonstrate that the synergy of two active sites, >B−O−O−B< and >B−O−B<, is crucial for the first and second H‐transfer, respectively. With the increase in molecular mass of the considered light alkanes, the ODH reaction temperature decreases. In the case of butane and isobutane, the ODH reaction occurs almost at the same temperature indicating that the reaction is independent of the shape of the isomer. The rate‐limiting nature of the first H‐transfer step is predicted. The charge redistribution during H‐transfers and localized oxygen atomic states in the conduction band are explored to suggest possible descriptors for the rational design of new catalysts. The universal action of the >B−O−O−B< and >B−O−B< active sites for ODH of the light alkanes paves the way for metal‐free BN‐based materials for future catalytic applications.
Lei, Y, Wu, C, Lu, X, Hua, W, Li, S, Liang, Y, Liu, H, Lai, W, Gu, Q, Cai, X, Wang, N, Wang, Y, Chou, S, Liu, H, Wang, G & Dou, S 2022, 'Streamline Sulfur Redox Reactions to Achieve Efficient Room‐Temperature Sodium–Sulfur Batteries', Angewandte Chemie International Edition, vol. 61, no. 16, p. e202200384.
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AbstractIt is vital to dynamically regulate S activity to achieve efficient and stable room‐temperature sodium–sulfur (RT/Na−S) batteries. Herein, we report using cobalt sulfide as an electron reservoir to enhance the activity of sulfur cathodes, and simultaneously combining with cobalt single atoms as double‐end binding sites for a stable S conversion process. The rationally constructed CoS2 electron reservoir enables the straight reduction of S to short‐chain sodium polysulfides (Na2S4) via a streamlined redox path through electron transfer. Meanwhile, cobalt single atoms synergistically work with the electron reservoir to reinforce the streamlined redox path, which immobilize in situ formed long‐chain products and catalyze their conversion, thus realizing high S utilization and sustainable cycling stability. The as‐developed sulfur cathodes exhibit a superior rate performance of 443 mAh g−1 at 5 A g−1 with a high cycling capacity retention of 80 % after 5000 cycles at 5 A g−1.
Li, J, Song, J, Luo, L, Zhang, H, Feng, J, Zhao, X, Guo, X, Dong, H, Chen, S, Liu, H, Shao, G, Anthopoulos, TD, Su, Y, Wang, F & Wang, G 2022, 'Synergy of MXene with Se Infiltrated Porous N‐Doped Carbon Nanofibers as Janus Electrodes for High‐Performance Sodium/Lithium–Selenium Batteries', Advanced Energy Materials, vol. 12, no. 32, pp. 2200894-2200894.
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AbstractMetal–selenium (M–Se) batteries are considered promising candidates for next‐generation battery technologies owing to their high energy density and high‐rate capability. However, Se cathode suffers from poor cycling performance and low Coulombic efficiency, owing to the shuttle effect of polyselenides. Herein, it is reported the incorporation of Ti3C2Tx MXene onto Se infiltrated porous N‐doped carbon nanofibers (PNCNFs) to construct free‐standing Janus PNCNFs/Se@MXene cathodes for high‐performance Na–Se and Li–Se batteries. The increase of pyrrolic‐N content and the porous structure of the PNCNFs is conducive to enhancing the adsorption of Na2Se and alleviating the shuttle effect. Meanwhile, density functional theory (DFT) calculations have proven that 2D Ti3C2Tx MXene with polar interfaces enables the effective chemical immobilization and physical blocking of polyselenides to suppress the shuttle effect. The unique architecture with Ti3C2Tx MXene built on top of interlinked nanofiber ensures the continuous electron transfer for redox reaction. As a result, the novel Janus PNCNFs/Se@MXene electrodes deliver robust rate capabilities and superior long‐term cycling stability in both Na–Se and Li–Se batteries. The incorporation of 2D MXene to construct Janus electrodes provides a competitive advantage for selenium‐based cathode materials and highlights a new strategy for developing high‐performance batteries.
Liu, S, Teng, Z, Liu, H, Wang, T, Wang, G, Xu, Q, Zhang, X, Jiang, M, Wang, C, Huang, W & Pang, H 2022, 'A Ce‐UiO‐66 Metal–Organic Framework‐Based Graphene‐Embedded Photocatalyst with Controllable Activation for Solar Ammonia Fertilizer Production', Angewandte Chemie, vol. 134, no. 37.
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AbstractCurrently, nitrogen fertilizers feed half of the global population, but their use is limited by energy consumption and transportation. Therefore, it is important to study photocatalysts for use in solar nitrogen fertilizers. Herein, a new type of graphene‐embedded Ce‐based UiO‐66 (Ce‐UiO‐66) photocatalyst (GSCe) is investigated. Ce‐UiO‐66 is activated by the breakage of benzene‐C bonds and the formation of active sites by ultraviolet light in water. Moreover, embedding graphene effectively controls activation and improves nitrogen fixation. GSCe exhibited a remarkable apparent quantum efficiency (AQE) of 9.25 % and stability under 365 nm light with solar‐level intensity. GSCe also performed well as a solar ammonia fertilizer for crop cultivation. This investigation opens up opportunities for nitrogen fixation photocatalysts to be used as environmentally friendly solar nitrogen fertilizers.
Long, MQ, Tang, KK, Xiao, J, Li, JY, Chen, J, Gao, H, Chen, WH, Liu, CT & Liu, H 2022, 'Recent advances on MXene based materials for energy storage applications', Materials Today Sustainability, vol. 19, pp. 100163-100163.
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McPherson, DJ, Dowd, A, Arnold, MD, Gentle, A & Cortie, MB 2022, 'Electrochemical energy storage on nanoporous copper sponge', Journal of Materials Research, vol. 37, no. 13, pp. 2195-2203.
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AbstractA proof-of-principle double-layer symmetrical supercapacitor with nanoporous copper/copper oxide electrodes and an aqueous electrolyte is investigated. The electrodes are manufactured by selective dissolution of Al from a eutectic composition of Cu17.5Al82.5using 5 M NaOH. The ostensible (i.e., net external) capacitance of a symmetrical two-electrode cell with 0.1 M KNO3electrolyte is assessed over a series of charge/discharge cycles and is about 2 F per gram of Cu in this simple prototype. Capacitance varies during a discharge cycle due evidently to the deeply buried surfaces and pseudocapacitive reactions contributing charge toward the end of a discharge cycle. In principle such a device should have very low ohmic losses due to its highly conductive backbone and would be suitable for applications requiring maximum energy efficiency over repeated cycling. The aqueous electrolyte ensures fire safety but this comes at the cost of lower energy content.Graphical abstract
Nazrul‐Islam, SMK, Rahman, MR, Ahmed, AJ, Yun, FF, Cortie, DL, Wang, X & Cortie, MB 2022, 'Beneficial Effect of Na2CO3 Additions on the Thermoelectric Performance of Melt‐Route Cu2Se', Advanced Electronic Materials, vol. 8, no. 3, pp. 2100802-2100802.
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AbstractHigh‐performance thermoelectric materials require simultaneous reduction of thermal conductivity and electrical resistivity, among other criteria. Here it is shown that the introduction of Na2CO3 into the melt‐route fabrication process for the well‐known thermoelectric Cu2Se has a beneficial and surprisingly strong effect. There is a significant enhancement in electrical conductivity which density functional theory calculations suggest may be due to the effect of Na and O doping in the Cu2Se matrix. There is also a 34% reduction in thermal conductivity which is likely due to a high density of defects causing scattering of phonons. Overall, however, there is only relatively a small change in Seebeck coefficient. A higher power factor of 12.6 µW cm−1 K−2 is achieved versus 8.8 µW cm−1 K−2 for standard Cu2Se. A very high value of zT of 2.3 is obtained at 804 K versus 1.1 for standard Cu2Se.
Nguyen, D-A, Tran, X-T, Dang, KN & Iacopi, F 2022, 'A low-power, high-accuracy with fully on-chip ternary weight hardware architecture for Deep Spiking Neural Networks', Microprocessors and Microsystems, vol. 90, pp. 104458-104458.
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Recently, Deep Spiking Neural Network (DSNN) has emerged as a promising neuromorphic approach for various AI-based applications, such as image classification, speech recognition, robotic control etc. on edge computing platforms. However, the state-of-the-art offline training algorithms for DSNNs are facing two major challenges. Firstly, many timesteps are required to reach comparable accuracy with traditional frame-based DNNs algorithms. Secondly, extensive memory requirements for weight storage make it impossible to store all the weights on-chip for DSNNs with many layers. Thus the inference process requires continue access to expensive off-chip memory, ultimately leading to performance degradation in terms of throughput and power consumption. In this work, we propose a hardware-friendly training approach for DSNN that allows the weights to be constrained to ternary format, hence reducing the memory footprints and the energy consumption. Software simulations on MNIST and CIFAR10 datasets have shown that our training approach could reach an accuracy of 97% for MNIST (3-layer fully connected networks) and 89.71% for CIFAR10 (VGG16). To demonstrate the energy efficiency of our approach, we have proposed a neural processing module to implement our trained DSNN. When implemented as a fixed, 3-layers fully-connected system, the system has reached at energy efficiency of 74nJ/image with a classification accuracy of 97% for MNIST dataset. We have also considered a scalable design to support more complex network topologies when we integrate the neural processing module with a 3D Network-on-Chip.
Payne, M, Bottomley, AL, Och, A, Hiscocks, HG, Asmara, AP, Harry, EJ & Ung, AT 2022, 'Synthesis and biological evaluation of tetrahydroisoquinoline-derived antibacterial compounds', Bioorganic & Medicinal Chemistry, vol. 57, pp. 116648-116648.
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Antibiotic resistance is one of the greatest threats to modern medicine. Drugs that were once routinely used to treat infections are being rendered ineffective, increasing the demand for novel antibiotics with low potential for resistance. Here we report the synthesis of 18 novel cationic tetrahydroisoquinoline-triazole compounds. Five of the developed molecules were active against S. aureus at a low MIC of 2-4 μg/mL. Hit compound 4b was also found to eliminate M. tuberculosis H37Rv at MIC of 6 μg/mL. This potent molecule was found to eliminate S. aureus effectively, with no resistance observed after thirty days of sequential passaging. These results identified compound 4b and its analogues as potential candidates for further drug development that could help tackle the threat of antibiotic resistance.
Qi, X-R, Liu, Y, Ma, L-L, Hou, B-X, Zhang, H-W, Li, X-H, Wang, Y-S, Hui, Y-Q, Wang, R-X, Bai, C-Y, Liu, H, Song, J-J & Zhao, X-X 2022, 'Delicate synthesis of quasi-inverse opal structural Na3V2(PO4)3/N-C and Na4MnV(PO4)3/N-C as cathode for high-rate sodium-ion batteries', Rare Metals, vol. 41, no. 5, pp. 1637-1646.
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Poor conductivity and sluggish Na+ diffusion kinetic are two major drawbacks for practical application of sodium super-ionic conductor (NASICON) in sodium-ion batteries. In this work, we report a simple approach to synthesize quasi-inverse opal structural NASICON/N-doped carbon for the first time by a delicate one-pot solution-freeze drying-calcination process, aiming at fostering the overall electrochemical performance. Especially, the quasi-inverse opal structural Na3V2(PO4)3/N-C (Q-NVP/N-C) displayed continuous pores, which provides interconnected channels for electrolyte permeation and abundant contacting interfaces between electrolyte and materials, resulting in faster kinetics of redox reaction and higher proportion of capacitive behavior. As a cathode material for sodium-ion batteries, the Q-NVP/N-C exhibits high specific capacity of 115 mAh·g−1 at 1C, still 61 mAh·g−1 at ultra-high current density of 100C, and a specific capacity of 89.7 mAh·g−1 after 2000 cycles at 20C. This work displays the general validity of preparation method for not only Q-NVP/N-C, but also Na4MnV(PO4)3, which provides a prospect for delicate synthesis of NASICON materials with excellent electrochemical performance. Graphical Abstract: [Figure not available: see fulltext.]
Rahman, MA, Ali, S, Phillips, MR & Ton-That, C 2022, 'Multi-wavelength emission through self-induced defects in GaZnO microrods', Journal of Alloys and Compounds, vol. 895, pp. 162693-162693.
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Multi-wavelength emission in wide bandgap semiconductors is commonly achieved through ternary alloying or quantum size effects. However, multi-wavelength emission within a single microstructure is highly challenging using these approaches. Here, we demonstrate that the luminescence wavelength within individual GaZnO microrods can be tailored via defect engineering. Fast chemical vapor growth of oxygen-rich ZnO microrods with Ga2O3 as an additive in the ZnO vapour leads to formation of a tapered morphology with graded distribution of Ga dopants, while the Ga incorporation does not significantly alter their crystal structure. With increasing Ga content from 1 to 6 at% from tip to base, the GaZnO microrods increase in diameter towards the substrate in accordance with the birth-and-spread mechanism. The local near-band-edge emission within single ZnO microrods, analyzed by nanoscale cathodoluminescence spectroscopy, exhibits a red shift of ~0.6 eV with increasing Ga content and exhibits signature characteristics of an excitonic emission. Density Functional Theory calculations reveal that the variation in the emission wavelength arises from bandgap narrowing due to the merging of the electronic states of Ga defect complexes with ZnO energy bands. The experimental and theoretical results demonstrate (i) the utility of using the self-regulation of defect compensation effects for band gap engineering and (ii) the possibility of multi-wavelength light sources within individual microrods.
Raza, A, Hassan, JZ, Mahmood, A, Nabgan, W & Ikram, M 2022, 'Recent advances in membrane-enabled water desalination by 2D frameworks: Graphene and beyond', Desalination, vol. 531, pp. 115684-115684.
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The growing population rate and expansion of industrial sector are associated with climate variation, which steered towards global water complications. The current review summarizes the next-generation hybrid graphene-based membrane materials for water cleansing to come across global freshwater supplies. In this regard, graphene-based membrane materials are assumed as innovative materials headed for desalination route owing to their tunable functionalities as well as atomic thickness. The discussion of operating conditions and production procedures of membrane on membrane fouling and separation mechanisms are described. Furthermore, its development merits, and limitations compared to traditional polymeric membranes are also discussed. This review discusses the use of 2D materials as building blocks for membrane structures, current developments in 2D-enabled membranes, and their prospects. More devotion is required for membrane selectivity and water permeability for long-term setup at environments alike with the field for performance examination; this helps to prolong applications of graphene-based membranes materials. In this regard, we summarized the research growth on 2D materials for membrane-based water desalination for more attention. Moreover, the design strategies containing layer-layer spacing and pore size optimization to sustain the constancy of the membranes are predominantly explained. Finally, present tasks and future research directions are also offered.
Ren, Z, Zhang, X, Huang, Z, Hu, J, Li, Y, Zheng, S, Gao, M, Pan, H & Liu, Y 2022, 'Controllable synthesis of 2D TiH2 nanoflakes with superior catalytic activity for low-temperature hydrogen cycling of NaAlH4', Chemical Engineering Journal, vol. 427, pp. 131546-131546.
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Nanosized titanium compounds are particularly effective in catalyzing hydrogen cycling by NaAlH4. Titanium hydride (TiH2), as a catalyst, is highly interesting since it contributes hydrogen in addition to active Ti. However, it has been challenging to fabricate nanosized TiH2 due to the strong affinity of Ti with oxygen. Herein, TiH2 nanoflakes with a lateral size of ~10 nm and thickness of ~1 nm are successfully synthesized through a novel facile one-pot solvothermal process. In an anhydrous THF solution, LiH reacts with TiCl4 rapidly at 100 °C forming TiH2 and LiCl. The newly formed TiH2 nucleates and grows epitaxially on the graphene surface due to the well-matched lattice parameters, giving rise to the formation of TiH2 nanoflakes. Both theoretical calculations and experiments reveal the generation of Cl· radicals and unsaturated C[dbnd]C bonds when TiCl4 reacts with THF, which promotes the formation of TiH2. The nanoflake-like TiH2 on graphene enables an outstanding hydrogen storage performance of NaAlH4, i.e., full dehydrogenation at 80 °C and hydrogenation at 30 °C and under 100 bar H2, with a practical hydrogen capacity of 4.9 wt%, which has been never reported before.
Sarker, PC, Guo, Y, Lu, H & Zhu, JG 2022, 'Improvement on parameter identification of modified Jiles-Atherton model for iron loss calculation', Journal of Magnetism and Magnetic Materials, vol. 542, pp. 168602-168602.
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The physical behaviour of a magnetic material can be characterized by Jiles-Atherton (J-A) model where some model parameters are generally identified by optimization techniques. For identification of model parameters using optimization techniques, an error criterion based on the error between the measured and calculated magnetic flux density (B) or magnetic field strength (H) is commonly considered where the relative error in the calculation of iron loss is ignored. Consequently, the calculated iron loss from B-H loop sometimes highly differs from its experimental value. In this paper, the error criteria for J-A model's parameter identification are designed as the combination of the relative iron loss error criterion and the general existing error criterion. Furthermore, a modified J-A model is proposed to improve the agreement between experimental and calculated results especially at the low magnetic induction levels by introducing a scaling factor in the anhysteretic magnetization. The proposed modified J-A model and the effectiveness of the error criteria for its parameter identification are tested by comparing calculated results with the experimental results as well as recently works in the literature.
Shabbir, B, Liu, J, Krishnamurthi, V, Ayyubi, RAW, Tran, K, Tawfik, SA, Hossain, MM, Khan, H, Wu, Y, Shivananju, BN, Sagar, RUR, Mahmood, A, Younis, A, Uddin, MH, Bukhari, SA, Walia, S, Li, Y, Spencer, MJS, Mahmood, N & Jasieniak, JJ 2022, 'Soft X‐ray Detectors Based on SnS Nanosheets for the Water Window Region', Advanced Functional Materials, vol. 32, no. 3, pp. 2105038-2105038.
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AbstractThe structural characteristics of biological specimens, such as wet proteins and fixed living cells, can be conveniently probed in their host aqueous media using soft X‐rays in the water window region (200–600 eV). Conventional X‐ray detectors in this area exhibit low spatial resolution, have limited sensitivity, and require complex fabrication procedures. Here, many of these limitations are overcome by introducing a direct soft X‐ray detector based on ultrathin tin mono‐sulfide (SnS) nanosheets. The distinguishing characteristic of SnS is its high photon absorption efficiency in the soft X‐ray region. This factor enables the fabricated soft X‐ray detectors to exhibit excellent sensitivity values on the order of at peak energies of ≈600 eV. The peak signal is found to be sensitive to the number of stacked SnS layers, with thicker SnS nanosheet assemblies yielding a peak response at higher energies and with peak sensitives of over 2.5 at 1 V. Detailed current–voltage and temporal characteristics of these detectors are also presented. These results showcase the excellent performance of SnS nanosheet‐based soft X‐ray detectors compared to existing direct soft X‐ray detectors, including that of the emerging organic–inorganic perovskite class of materials.
Sharif, HMA, Ali, M, Mahmood, A, Asif, MB, Din, MAU, Sillanpää, M, Mahmood, A & Yang, B 2022, 'Separation of Fe from wastewater and its use for NOx reduction; a sustainable approach for environmental remediation', Chemosphere, vol. 303, no. Pt 2, pp. 135103-135103.
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The nitrogen and sulphur oxide (NOx and SO2) emissions are causing a serious threat to the existence of life on earth, requiring their effective removal for a sustainable future. Among various approaches, catalytic or electrochemical reduction of air pollutants (NOx) has gained much attention due to its high efficiency and the possibility of converting these gases into valuable products. However, the required catalysts are generally synthesized from lab-grade chemicals, which may not be a sustainable approach. Herein, a sustainable approach is presented to synthesize an efficient iron-based catalyst directly from industrial/lake wastewater (WW) for NOx-reduction. According to the theoretical calculations and experimental results, Fe-ions could be readily recovered from wastewater because it has the best adsorption efficiency among all other co-existing metals (Ni2+, Cd2+, Co2+, Cu2+, and Cr6+). The subsequent experimental investigations confirmed the preferential Fe adsorption from different WW streams to develop Fe3O4@EDTA-Fe composite, whereby Fe3O4 could be used due to its high recycling ability, and ethylenediaminetetraacetic acid (EDTA) acted as a chelating agent to adsorb Fe-metal from effluents. The Fe3O4@EDTA-Fe exhibited high efficiency (≥87%) for NOx reduction even in the presence of high-degree oxygen contents (10-12%). Moreover, Fe3O4-EDTA-Fe showed excellent long-term stability for 24 h and maintained more than 80% NOx reduction. The fabricated catalyst has a great potential for executing a dual role simultaneously for Fe-recovery and NOx removal, promoting the circular economy concept and providing a potentially sustainable remediation approach for large-scale applications.
Shi, Y-L, Huang, D, Ling, FC-C, Tian, Q-S, Liao, L-S, Phillips, MR & Ton-That, C 2022, 'Correlation between small polaron tunneling relaxation and donor ionization in Ga2O3', Applied Physics Letters, vol. 120, no. 17, pp. 172105-172105.
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Pulsed laser deposition is employed to fabricate as-grown amorphous and post-growth annealed crystalline β-Ga2O3 films. The films annealed at temperatures above 600 °C are found to exhibit a pure monolithic phase with a bandgap of 4.7 eV. The thermally activated donor ionization and dielectric relaxation of these films are systematically investigated by temperature-dependent DC and AC conductivity measurements, and complex electric modulus analysis. A donor level at ∼180 meV below the conduction band edge and a small polaron tunneling (SPT) relaxation with an activation energy of ∼180 meV are observed in the as-grown amorphous Ga2O3 film but not in the monolithic β-Ga2O3 film. The SPT occurs between donor sites with its thermal relaxation of polarization being associated with the thermal ionization of the donor state. Thermal annealing of the amorphous films removes the 180 meV donors as well the corresponding SPT relaxation.
Shirazi, RS, Vyssotski, M, Lagutin, K, Thompson, D, MacDonald, C, Luscombe, V, Glass, M, Parker, K, Gowing, EK, Williams, DBG & Clarkson, AN 2022, 'Neuroprotective activity of new Δ3‐N‐acylethanolamines in a focal ischemia stroke model', Lipids, vol. 57, no. 1, pp. 17-31.
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AbstractN‐acylethanolamines (NAE, also called ethanolamides) are significant lipid signaling molecules with anti‐inflammatory, pain‐relieving, cell‐protective, and anticancer properties. Here, we present the use of a hitherto unreported group of Δ3‐NAE and also some Δ4‐ and Δ5‐NAE, in in vitro and in vivo assays to gain a better understanding of their structure–bioactivity relationships. We have developed an efficient synthetic method to rapidly produce novel unlabeled and 13C‐labeled Δ3‐NAE (NAE‐18:5n‐3, NAE‐18:4n‐6) and Δ4‐NAE (NAE‐22:5n‐6). The new NAE with shorter carbon backbone structures confers greater neuroprotection than their longer carbon backbone counterparts, including anandamide (Δ5‐NAE‐20:4n‐6) in a focal ischemia mouse model of stroke. This study highlights structure‐dependent protective effects of new NAE following focal ischemia, in which some of the new NAE, administered intranasally, lead to significantly reduced infarct volume and improved recovery of limb use. The relative affinity of the new NAE toward cannabinoid receptors was assessed against anandamide, NAE‐22:6n‐3 and NAE‐20:5n‐3, which are known cannabinoid receptor ligands with high‐binding constants. Among the newly synthesized NAE, Δ4‐NAE‐22:5n‐6 shows the greatest relative affinity to cannabinoid receptors hCB1 and hCB2, and inhibition of cyclic adenosine monophosphate activity through hCB2 compared to anandamide.
Sillapachaiyaporn, C, Chuchawankul, S, Nilkhet, S, Moungkote, N, Sarachana, T, Ung, AT, Baek, SJ & Tencomnao, T 2022, 'Ergosterol isolated from cloud ear mushroom (Auricularia polytricha) attenuates bisphenol A-induced BV2 microglial cell inflammation', Food Research International, vol. 157, pp. 111433-111433.
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Song, A, Tian, H, Yang, W, Yang, W, Xie, Y, Liu, H, Wang, G & Shao, G 2022, 'Enhanced confinement synthesis of atomically dispersed Fe-N-C catalyst from resin polymer for oxygen reduction', Journal of Energy Chemistry, vol. 65, pp. 630-636.
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Due to larger atom utilization, unique electronic properties and unsaturated coordination, atomically dispersed non-precious metal catalysts with outstanding performances have received great attention in electrocatalysis. Considering the challenge of serious aggregation, rational synthesis of an atomic catalyst with good dispersion of atoms is paramount to the development of these catalysts. Herein, we report an enhanced confinement strategy to synthesize a catalyst comprised of atomically dispersed Fe supported on porous nitrogen-doped graphitic carbon from the novel and more cross-linkable Melamine-Glyoxal Resin. Densified isolated grid trapping, excessive melamine restricting, and nitrogen anchoring are strongly combined to ensure the final atomic-level dispersion of metal atoms. Experimental studies revealed enhanced kinetics of the obtained catalyst towards oxygen reduction reaction (ORR). This catalytic activity originates from the highly active surface with atomically dispersed iron sites as well as the multi-level three-dimensional structure with fast mass and electron transfer. The enhanced confinement strategy endows the resin-derived atomic catalyst with a great prospect to develop for commercialization in future.
Su, D 2022, 'Powerful qua-functional electrolyte additive for lithium metal batteries', Green Energy & Environment, vol. 7, no. 3, pp. 361-364.
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Lithium metal batteries (LMBs) have attracted tremendous research attention because of the high theoretical capacity (3860 mAh g−1) and the lowest electrochemical potential (−3.04 V vs standard hydrogen electrode). However, the Lithium dendrites, forming from plating/stripping processes, cause the excessive consumption of electrolyte and active Li and the puncture on the separator. This limits the commercialization of LMBs. Recently, Ma's group proposed heptafluorobutyric anhydride (HFA) as qua-functional electrolyte additive and verified the protection mechanism from the structure and electrochemical properties. Such results creatively put forward qua-functional electrolyte additive for the improvement of LMBs and provides good experience for the exploration of multi-functional additive, inspiring researchers to explore new multi-functional electrolyte additives in future.
Tai, MC, Arnold, MD, Estherby, C, de Silva, KSB, Gentle, AR, Cortie, DL, Mitchell, DRG, Westerhausen, MT & Cortie, MB 2022, 'Spontaneous Emergence of Optically Polarizing Nanoscale Structures by Co-Deposition of Aluminum with Refractory Metals: Implications for High-Temperature Polarizers', ACS Applied Nano Materials, vol. 5, no. 3, pp. 4316-4324.
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The unexpected growth of highly aligned and optically polarizing metallic fins during physical vapor deposition under modestly oblique conditions is investigated. The fins exhibit nanoscale dimensions and are formed when Al is co-sputtered with any of V, Cr, Nb, Mo, Ta, W, Ru, Fe, Ni, Pt, Zr, Mg, and Ti. It is proposed that the phenomenon is caused by anomalously low atomic mobility in the alloys and intermetallic compounds formed by co-depositing with Al. In contrast, when Cu, Ag, and Au (which diffuse more rapidly in Al) are deposited, no fins form. There is a sharp visible transition in optical properties as the ratio of Al to other element is decreased: the color of the sample changes from black to silver-white for compositions containing less than about 55 atom % Al. The region over which the color change occurs is associated with a very strongly polarized reflectance. Cross-sectional elemental mapping and Monte Carlo simulations suggest that growth of the fins may be nucleated by Al hillocks and enhanced by shadowing effects. The diversity of suitable metals makes this a versatile technique for producing nanoscale polarizing surfaces suitable for high-flux and high-temperature applications.
Tang, K, Gao, H, Xiao, J, Long, M, Chen, J, Liu, H & Wang, G 2022, 'Hierarchical Oα-rich Co3O4 nanoarray anchored on Ni foam with superior lithiophilicity enabling ultrastable lithium metal batteries', Chemical Engineering Journal, vol. 436, pp. 134698-134698.
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Lithium metal batteries (LMBs) are considered as the ultimate choice in the next-generation high performance energy-storage systems due to their outstanding theoretical energy density (≥500 Wh kg−1). However, the unavoidable dendrite issues and infinite volume change during repeated plating/stripping induce poor electrochemical performance and serious safety issues. Here, we designed and prepared an integrated Oα (O- or O22–)-rich Co3O4 nanoarrays anchored on Ni foam (Oα-Co3O4@NF) scaffold as a stable host for ultra-fast lithium metal infusion. Remarkably, the highly reactive Oα behaves low energy bonding and strong electron affinity, which are further verified by the results of density functional theory, giving rise to high lithiophilicity and inhibiting the dendrites formation effectively. Moreover, the by-product NiO formed on the NF during the calcination process combines with Oα-Co3O4 to display superior dual-wettability toward molten Li. As a result, the Oα-Co3O4@NF electrode achieves a Coulombic efficiency above 99.00% more than 450 cycles at a current density of 1 mA cm−2, and the Oα-Co3O4@NF-Li anode presents a super-long and stable lifetime of 800 h during the repeated plating/striping process. When coupled with a high-loading LiFePO4 cathode, the full cells deliver excellent rate capability and 88.96% capacity retention after 200 cycles under 0.5C.
Tareen, AK, Khan, K, Iqbal, M, Golovynskyi, S, Zhang, Y, Mahmood, A, Mahmood, N, Long, J, Al-Ghamdi, A, Li, C & Zhang, H 2022, 'Recent advances in MXenes: new horizons in biomedical technologies', Materials Today Chemistry, vol. 26, pp. 101205-101205.
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Tareen, AK, Khan, K, Iqbal, M, Zhang, Y, Long, J, Mahmood, A, Mahmood, N, Xie, Z, Li, C & Zhang, H 2022, 'Recent advance in two-dimensional MXenes: New horizons in flexible batteries and supercapacitors technologies', Energy Storage Materials, vol. 53, pp. 783-826.
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MXenes (two dimensional (2D) transition metal (TM) carbides (TMCs), TM nitrides (TMNs), and TM carbonitrides (TMCNs) are emerged as future biggest 2D materials (2DMs) family with novel applications in different nanotechnological research in academic as well as industrial level. MXenes NMs have the potential to be classified as a “wonder material” in the category of 2D nanomaterials (NMs). MXenes were studied and synthesized for over a decade since their first discovery in 2011, and till now more than 50 members are experimentally studied and more than 100 are theoretically investigated. Synthesis techniques are not restricted to the first introduced top-down HF based etching method but new innovative synthesis methods, such as, water (H2O)-free etching, molten salts etching and bottom-up method, like Chemical vapor deposition (CVD) method etc were also studied, providing multifunctional surface chemistry based MXenes NMs with novel configuration, and desirable characteristics. MXenes are used as important components in a number of flexible energy storage devices (FESDs), for instance secondary batteries, supercapacitors (SCs), Micro-SCs (MSCs) and Micro-batteries (MBs), etc due to their distinctive layered structures, high electrochemical performance and fascinating functional capabilities. In this review, we first will discuss in detail the MXenes NMs synthesis methods, secondly selected properties, and third their applications in various FESDs. After that, we will summarize and discuss the most present problems associated with MXenes NMs synthesis and their applications in FESDs, and possible solutions to those problems. Finally we will discuss the presents interesting vision for the future progress of the MXenes-based NMs in wearable and FESDs, their limitations, and suggestions.
Tareen, AK, Khan, K, Iqbal, M, Zhang, Y, Long, J, Nazeer, F, Mahmood, A, Mahmood, N, Shi, Z, Ma, C, Huan, W, Khan, MF, Yin, J, Li, C & Zhang, H 2022, 'Recent advances in novel graphene: new horizons in renewable energy storage technologies', Journal of Materials Chemistry C, vol. 10, no. 32, pp. 11472-11531.
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Graphene based supercapacitors and batteries are a highly competitive choice for electrochemical energy storage devices, thanks to their ultrahigh power density, improved rate capability, long-term cyclability, and remarkable safety.
Tareen, AK, Khan, K, Iqbal, M, Zhang, Y, Xie, Z, Mahmood, A, Mahmood, N, Long, J, Li, C & Zhang, H 2022, 'Recent major advances and challenges in the emerging graphene-based nanomaterials in electrocatalytic fuel cell technology', Journal of Materials Chemistry C, vol. 10, no. 47, pp. 17812-17873.
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Graphene and its derivatives with unique chemical and physical features have motivated great efforts and achieved substantial advances in fuel cell applications for renewable energy production.
Usman, M, Ahsan, MT, Javed, S, Ali, Z, Zhan, Y, Ahmed, I, Butt, S, Islam, M, Mahmood, A & Akram, MA 2022, 'Facile synthesis of iron nickel cobalt ternary oxide (FNCO) mesoporous nanowires as electrode material for supercapacitor application', Journal of Materiomics, vol. 8, no. 1, pp. 221-228.
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Wang, N, Yao, H, Tao, Q, Sun, J, Ma, H, Wang, Y, Zhou, C, Fan, H, Shao, H, Qin, A, Su, D, Wang, C & Chong, H 2022, 'TPE based aggregation induced emission fluorescent sensors for viscosity of liquid and mechanical properties of hydrogel', Chinese Chemical Letters, vol. 33, no. 1, pp. 252-256.
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Two amphiphilic TPE E/Z isomers with aggregation induced emission (AIE) property have been synthesized and characterized. The logarithmic fluorescent intensity of the two molecules was in positive relationship with logarithmic viscosity of liquid. To note, the Z-TPE isomer exhibited more sensitivity in the viscosity of liquid sensing in comparison with the corresponding E-TPE counterpart (around 1.80 folds). Furthermore, two molecules could be used as fluorescent sensors for mechanical properties (viscosity and storage modulus) of hydrogel as well. In addition, two sensors displayed low cytotoxicity in normal tissue cell line (L929) within the concentration range of 2–10 µmol/L. These results potentially promised their applications as fluorescent sensors for mechanical properties in the fields of biological and biomedical.
Wang, S, Lu, J, Li, B, Liu, C, Wang, Y, Lei, G, Guo, Y & Zhu, J 2022, 'Design and analysis of mechanical flux-weakening device of axial flux permanent magnet machines', Journal of Power Electronics, vol. 22, no. 4, pp. 653-663.
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Due to the low inductance of an axial flux permanent magnet machine (AFPMM), the constant power speed regulation range is small. A new mechanical flux-weakening method for single-rotor single-stator AFPMMs is proposed in this paper. By installing a mechanical flux-weakening device on one side of the stator and rotating it certain angle, the speed regulation of the flux-weakening can be realized. The device is simple in structure, easy to operate, and can be operated in the process of machine operation. The validity of the device is verified by applying it to a machine. Finite-element software is used to calculate and analyze the performances of two machines with the device.
Wang, S, Zhao, S, Guo, X & Wang, G 2022, '2D Material‐Based Heterostructures for Rechargeable Batteries', Advanced Energy Materials, vol. 12, no. 4, pp. 2100864-2100864.
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Abstract2D materials are regarded as promising electrode materials for rechargeable batteries because of their advantages in providing ample active sites and improving electrochemical reaction kinetics. However, it remains a great challenge for 2D materials to fulfill all requirements for high‐performance energy storage devices in terms of electronic conductivity, the number of accessible active sites, structural stability, and mass production capability. Recent advances in constructing 2D material‐based heterostructures offer opportunities for utilizing synergistic effects between the individual blocks to achieve optimized properties and enhanced performance. In this perspective, the latest advances of 2D material‐based heterostructures are summarized, with particular emphasis on their multifunctional roles in high‐performance rechargeable batteries. Synthetic strategies, structural features in mixed dimensionalities, structure engineering strategies, and distinct functionalities of the 2D material‐based heterostructures in various electrochemical applications are systematically introduced. Finally, challenges and perspectives are presented to highlight future opportunities for developing 2D material‐based heterostructures for practical energy storage.
Wang, T, He, D, Yao, H, Guo, X, Sun, B & Wang, G 2022, 'Development of Proteins for High‐Performance Energy Storage Devices: Opportunities, Challenges, and Strategies', Advanced Energy Materials, vol. 12, no. 44, pp. 2202568-2202568.
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AbstractIn pursuit of reducing environmental impact during battery manufacture, the utilization of nontoxic and renewable materials is essential for building a sustainable future. As one of the most intensively investigated biomaterials, proteins have recently been applied in various high‐performance rechargeable batteries. In this review, the opportunities and challenges of using protein‐based materials for high‐performance energy storage devices are discussed. Recent developments of directly using proteins as active components (e.g., electrolytes, separators, catalysts or binders) in rechargeable batteries are summarized. The advantages and disadvantages of using proteins are compared with the traditional counterparts, and the working mechanisms when using proteins to improve the electrochemical performances of rechargeable batteries are elucidated. Finally, the future development of applying biomaterials to build better batteries is predicted.
Wang, Y, Cui, X, Zhang, J, Qiao, J, Huang, H, Shi, J & Wang, G 2022, 'Advances of atomically dispersed catalysts from single-atom to clusters in energy storage and conversion applications', Progress in Materials Science, vol. 128, pp. 100964-100964.
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Owing to the special structural characteristics and maximized efficiency, atomically dispersed catalysts (ADCs) with different atom sizes ranged from the single atom to clusters can bridge the gap between heterogeneous and homogeneous catalysis. Tremendous progress has been made in ADCs including developing advanced synthesis strategies, promoting electrochemical performance and unraveling the underlying fundamental mechanisms. Herein, the recent progress of ADCs ranged from single-atom to clusters has been systematically reviewed with emphasis on key issues of synthesis methods, stabilization strategies, performance evaluation, mechanistic understanding, integrated experimental and theoretical studies in typical applications of energy storage and conversion, including oxygen reduction reaction in fuel cell and metal-air battery, oxygen evolution and hydrogen evolution reactions in water splitting, hydrogen oxidation reactions, carbon dioxide reduction and nitrogen reduction reaction. Centering on the topics, the most up-to-date results are present, along with the perspectives and challenges for the future development of ADCs.
Wu, C, Lei, Y, Simonelli, L, Tonti, D, Black, A, Lu, X, Lai, W, Cai, X, Wang, Y, Gu, Q, Chou, S, Liu, H, Wang, G & Dou, S 2022, 'Continuous Carbon Channels Enable Full Na‐Ion Accessibility for Superior Room‐Temperature Na–S Batteries', Advanced Materials, vol. 34, no. 8, pp. e2108363-2108363.
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AbstractPorous carbon has been widely used as an efficient host to encapsulate highly active molecular sulfur (S) in Li–S and Na–S batteries. However, for these sub‐nanosized pores, it is a challenge to provide fully accessible sodium ions with unobstructed channels during cycling, particularly for high sulfur content. It is well recognized that solid interphase with full coverage over the designed architectures plays critical roles in promoting rapid charge transfer and stable conversion reactions in batteries, whereas constructing a high‐ionic‐conductivity solid interphase in the pores is very difficult. Herein, unique continuous carbonaceous pores are tailored, which can serve as multifunctional channels to encapsulate highly active S and provide fully accessible pathways for sodium ions. Solid sodium sulfide interphase layers are also realized in the channels, showing high Na‐ion conductivity toward stabilizing the redox kinetics of the S cathode during charge/discharge processes. This systematically designed carbon‐hosted sulfur cathode delivers superior cycling performance (420 mAh g−1 at 2 A g−1 after 2000 cycles), high capacity retention of ≈90% over 500 cycles at current density of 0.5 A g−1, and outstanding rate capability (470 mAh g−1 at 5 A g−1) for room‐temperature sodium–sulfur batteries.
Wu, J, Tian, Y, Gao, Y, Gao, Z, Meng, Y, Wang, Y, Wang, X, Zhou, D, Kang, F, Li, B & Wang, G 2022, 'Rational Electrolyte Design toward Cyclability Remedy for Room‐Temperature Sodium–Sulfur Batteries', Angewandte Chemie International Edition, vol. 61, no. 30, p. e202205416.
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AbstractRechargeable room‐temperature sodium–sulfur (RT Na–S) batteries are a promising energy storage technology, owing to the merits of high energy density and low cost. However, their electrochemical performance has been severely hindered by the poor compatibility between the existing electrolytes and the electrodes. Here, we demonstrate that an all‐fluorinated electrolyte, containing 2,2,2‐trifluoro‐N,N‐dimethylacetamide (FDMA) solvent, 1,1,2,2‐tetrafluoroethyl methyl ether (MTFE) anti‐solvent and fluoroethylene carbonate (FEC) additive, can greatly enhance the reversibility and cyclability of RT Na–S batteries. A NaF‐ and Na3N‐rich cathode electrolyte interphase derived from FDMA and FEC enables a “quasi‐solid‐phase” Na–S conversion, eliminating the shuttle of polysulfides. The MTFE not only reduces polysulfide dissolution, but also further stabilizes the Na anode via a tailored solvation structure. The as‐developed RT Na–S batteries deliver a high capacity, long lifespan, and enhanced safety.
Wu, J, Tian, Y, Gao, Y, Gao, Z, Meng, Y, Wang, Y, Wang, X, Zhou, D, Kang, F, Li, B & Wang, G 2022, 'Rational Electrolyte Design toward Cyclability Remedy for Room‐Temperature Sodium–Sulfur Batteries', Angewandte Chemie, vol. 134, no. 30.
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AbstractRechargeable room‐temperature sodium–sulfur (RT Na–S) batteries are a promising energy storage technology, owing to the merits of high energy density and low cost. However, their electrochemical performance has been severely hindered by the poor compatibility between the existing electrolytes and the electrodes. Here, we demonstrate that an all‐fluorinated electrolyte, containing 2,2,2‐trifluoro‐N,N‐dimethylacetamide (FDMA) solvent, 1,1,2,2‐tetrafluoroethyl methyl ether (MTFE) anti‐solvent and fluoroethylene carbonate (FEC) additive, can greatly enhance the reversibility and cyclability of RT Na–S batteries. A NaF‐ and Na3N‐rich cathode electrolyte interphase derived from FDMA and FEC enables a “quasi‐solid‐phase” Na–S conversion, eliminating the shuttle of polysulfides. The MTFE not only reduces polysulfide dissolution, but also further stabilizes the Na anode via a tailored solvation structure. The as‐developed RT Na–S batteries deliver a high capacity, long lifespan, and enhanced safety.
Xu, J, Jin, Y, Liu, K, Lyu, N, Zhang, Z, Sun, B, Jin, Q, Lu, H, Tian, H, Guo, X, Shanmukaraj, D, Wu, H, Li, M, Armand, M & Wang, G 2022, 'A green and sustainable strategy toward lithium resources recycling from spent batteries', Science Advances, vol. 8, no. 40, p. eabq7948.
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Recycling lithium from spent batteries is challenging because of problems with poor purity and contamination. Here, we propose a green and sustainable lithium recovery strategy for spent batteries containing LiFePO 4 , LiCoO 2 , and LiNi 0.5 Co 0.2 Mn 0.3 O 2 electrodes. Our proposed configuration of “lithium-rich electrode || LLZTO@LiTFSI+P3HT || LiOH” system achieves double-side and roll-to-roll recycling of lithium-containing electrode without destroying its integrity. The LiTFSI+P3HT-modified LLZTO membrane also solves the H + /Li + exchange problem and realizes a waterproof protection of bare LLZTO in the aqueous working environment. On the basis of these advantages, our system shows high Li selectivity (97%) and excellent Faradaic efficiency (≥97%), achieving high-purity (99%) LiOH along with the production of H 2 . The Li extraction processes for spent LiFePO 4 , LiNi 0.5 Co 0.2 Mn 0.3 O 2 , and LiCoO 2 batteries is shown to be economically feasible. Therefore, this study provides a previously unexplored technology with low energy consumption as well as high economic and environmental benefits to realize sustainable lithium recycling from spent batteries.
Xu, J, Lv, W, Yang, W, Jin, Y, Jin, Q, Sun, B, Zhang, Z, Wang, T, Zheng, L, Shi, X, Sun, B & Wang, G 2022, 'In Situ Construction of Protective Films on Zn Metal Anodes via Natural Protein Additives Enabling High-Performance Zinc Ion Batteries', ACS Nano, vol. 16, no. 7, pp. 11392-11404.
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The strong activity of water molecules causes a series of parasitic side reactions on Zn anodes in the aqueous electrolytes. Herein, we introduce silk fibroin (SF) as a multifunctional electrolyte additive for aqueous zinc-ion (Zn-ion) batteries. The secondary structure transformation of SF molecules from α-helices to random coils in the aqueous electrolytes allows them to break the hydrogen bond network among free water molecules and participate in Zn2+ ion solvation structure. The SF molecules released from the [Zn(H2O)4(SF)]2+ solvation sheath appear to be gradually adsorbed on the surface of Zn anodes and in situ form a hydrostable and self-healable protective film. This SF-based protective film not only shows strong Zn2+ ion affinity to promote homogeneous Zn deposition but also has good insulating behavior to suppress parasitic reactions. Benefiting from these multifunctional advantages, the cycle life of the Zn||Zn symmetric cells reaches over 1600 h in SF-containing ZnSO4 electrolytes. In addition, by adopting a potassium vanadate cathode, the full cell shows excellent cycling stability for 1000 cycles at 3 A g-1. The in situ construction of a protective film on the Zn anode from natural protein molecules provides an effective strategy to achieve high-performance Zn metal anodes for Zn-ion batteries.
Yamamura, K, Zhu, L, Irvine, CP, Scott, JA, Singh, M, Jallandhra, A, Bansal, V, Phillips, MR & Ton-That, C 2022, 'Defect Compensation in Nitrogen-Doped β-Ga2O3 Nanowires: Implications for Bipolar Nanoscale Devices', ACS Applied Nano Materials, vol. 5, no. 9, pp. 12087-12094.
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Nitrogen (N) is a promising candidate currently being pursued for p-type doping in Ga2O3. In this work, the results of detailed investigations into N-doped β-Ga2O3nanowires using microstructural, chemical, and optical analyses are described. Monoclinic β-Ga2O3nanowires are grown by chemical vapor deposition using a metallic gallium (Ga) precursor and subsequently doped with N by remote plasma by exploiting their nanoscale cross sections and large surface-to-volume ratios. The N incorporation into β-Ga2O3is confirmed by X-ray absorption near-edge and Raman spectroscopies without changes in the nanowire morphology. N is found to exist mainly as molecular N2and N-O chemical states, but a significant portion of N substitutes on oxygen (O) sites. Concurrent temperature-resolved cathodoluminescence measurements of the undoped and N-doped β-Ga2O3are used to track the temperature dependences of their intrinsic ultraviolet (UV) luminescence and defect-related visible bands from 80 to 480 K. The blue and green bands increase in intensity relative to the UV after N doping; however, their intensity variations with temperature are found to be identical for the undoped and N-doped β-Ga2O3, indicating that these bands originate from existing recombination pathways in Ga2O3rather than from radiative N-related centers. The enhancement in defect-related luminescence in N-doped β-Ga2O3is explained by an increase in the concentration of O vacancies as a result of the compensation of NOacceptors.
Yang, Y, Liu, S, Dong, Z, Huang, Z, Lu, C, Wu, Y, Gao, M, Liu, Y & Pan, H 2022, 'Hierarchical conformal coating enables highly stable microparticle Si anodes for advanced Li-ion batteries', Applied Materials Today, vol. 26, pp. 101403-101403.
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Microsized silicon powders have great potential for high capacity anode materials in next-generation lithium ion batteries, because of the high gravimetric and volumetric energy densities, ease of mass production and low costs. However, large volume change and consequently rapid capacity fading upon lithiation and delithiation prevent its practical applications. Herein, we demonstrate an effective hierarchical conformal coating strategy for high-performance microsized Si anodes. The Si-based composites consist of an amorphous Li-Si-O inner coating layer and a graphene outer encapsulation layer, which are prepared by coupling reactive milling with electrostatic self-assembly. This unique hierarchical conformal coating structure not only strengthens the mechanical property (31.8 GPa for the elastic modulus) and promotes the ionic diffusion (2.03 × 10−10 cm2 s−1) of Si anode, but also effectively stabilizes the electrode/electrolyte interfaces and increases the electronic conductivity. As a result, a high reversible capacity (1450 mA⋅h g−1 at 0.1 A g−1), good cycling stability (97.7% of capacity retention from the 2nd to the 310th cycle at 0.5 A g−1), and high rate capability (703 mA⋅h g−1 at 5 A g−1) have been successfully achieved. These findings provide new insights into the improvement of electrochemical properties of microsized Si composite anodes for high-performance Li-ion batteries.
Yousaf, M, Naseer, U, Ali, I, Li, Y, Aftab, W, Mahmood, A, Mahmood, N, Gao, P, Jiang, Y & Guo, S 2022, 'Role of binary metal chalcogenides in extending the limits of energy storage systems: Challenges and possible solutions', Science China Materials, vol. 65, no. 3, pp. 559-592.
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Yousaf, M, Naseer, U, Imran, A, Li, Y, Aftab, W, Mahmood, A, Mahmood, N, Zhang, X, Gao, P, Lu, Y, Guo, S, Pan, H & Jiang, Y 2022, 'Visualization of battery materials and their interfaces/interphases using cryogenic electron microscopy', Materials Today, vol. 58, pp. 238-274.
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Zakria, M, Rogers, DJ, Scola, J, Zhu, L, Lockrey, M, Bove, P, Sandana, EV, Teherani, FH, Phillips, MR & Ton-That, C 2022, 'Two-dimensional confinement of excitons at the interface in nonpolar MgZnO/ZnO heterostructures', Physical Review Materials, vol. 6, no. 3.
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We report on the polarity-dependent excitonic emission at the interface in MgZnO/ZnO heterostructures grown on both polar and nonpolar ZnO single-crystal substrates. Structural and morphological analyses confirm that the heterostructures grow homoepitaxially on nonpolar m-plane and a-plane crystal substrates. The nonpolar heterostructures are investigated by depth-resolved cathodoluminescence spectroscopy revealing an excitonic interface emission centered at 3.12 eV, identified as the H-band signature of indirect excitons. These results reveal the formation of robust indirect excitons confined at the MgZnO/ZnO interface due to the presence of an epitaxially strained interfacial layer near the interface in the MgZnO, which is confirmed by high-order X-ray diffraction. It is also found that the H-band emission originates from the self-absorption of the ZnO free exciton emission in the proximity of the interface. Temperature-dependent studies of the H band yields a thermal activation energy of 47 meV for the indirect exciton in the nonpolar heterojunctions. This activation energy is the largest among all free and bound excitons in ZnO and is much higher than the values found in AlGaN/GaN and MgZnO/ZnO/sapphire hetrostructures. Our findings indicate that the optical properties of nonpolar heterostructures are strongly influenced by the piezoelectric effect.
Zhang, H, Song, J, Li, J, Feng, J, Ma, Y, Ma, L, Liu, H, Qin, Y, Zhao, X & Wang, F 2022, 'Interlayer-Expanded MoS2 Nanoflowers Vertically Aligned on MXene@Dual-Phased TiO2 as High-Performance Anode for Sodium-Ion Batteries', ACS Applied Materials & Interfaces, vol. 14, no. 14, pp. 16300-16309.
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Zhang, J, Zhao, Y, Sun, B, Xie, Y, Tkacheva, A, Qiu, F, He, P, Zhou, H, Yan, K, Guo, X, Wang, S, McDonagh, AM, Peng, Z, Lu, J & Wang, G 2022, 'A long-life lithium-oxygen battery via a molecular quenching/mediating mechanism', Science Advances, vol. 8, no. 3, p. eabm1899.
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The advancement of lithium-oxygen (Li-O 2 ) batteries has been hindered by challenges including low discharge capacity, poor energy efficiency, severe parasitic reactions, etc. We report an Li-O 2 battery operated via a new quenching/mediating mechanism that relies on the direct chemical reactions between a versatile molecule and superoxide radical/Li 2 O 2 . The battery exhibits a 46-fold increase in discharge capacity, a low charge overpotential of 0.7 V, and an ultralong cycle life >1400 cycles. Featuring redox-active 2,2,6,6-tetramethyl-1-piperidinyloxy moieties bridged by a quenching-active perylene diimide backbone, the tailor-designed molecule acts as a redox mediator to catalyze discharge/charge reactions and serves as a reusable superoxide quencher to chemically react with superoxide species generated during battery operation. The all-in-one molecule can simultaneously tackle issues of parasitic reactions associated with superoxide radicals, singlet oxygen, high overpotentials, and lithium corrosion. The molecular design of multifunctional additives combining various capabilities opens a new avenue for developing high-performance Li-O 2 batteries.
Zhang, X, Zhang, W, Zhang, L, Huang, Z, Hu, J, Gao, M, Pan, H & Liu, Y 2022, 'Single-pot solvothermal strategy toward support-free nanostructured LiBH4 featuring 12 wt% reversible hydrogen storage at 400 °C', Chemical Engineering Journal, vol. 428, pp. 132566-132566.
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Lithium borohydride (LiBH4) exhibits poor hydrogen storage reversibility because of phase separation between LiH and B due to foaming during thermal dehydrogenation. Herein, we report that by synthesizing nanostructured LiBH4 without any supports, the foaming and phase separation can be effectively suppressed, and consequently, the hydrogen storage reversibility of LiBH4 can be considerably improved. Using a facile single-pot solvothermal approach, a hierarchical porous nanostructured LiBH4 composed of 50–60 nm-sized primary nanoparticles is synthesized. The resulting neat nano-LiBH4 reversibly desorbs and absorbs approximately 12 wt% of H at 400 °C and under 100 bar H2. The superior hydrogen storage performance is attributed to the effective inhibition of foaming upon heating. The formation of LiH and B prior to melting, which can be associated with the largely reduced particle sizes and porous agglomeration structure, plays a crucial role in suppressing foaming. Our findings offer a new strategy for the preparation of nanoscaled freestanding borohydrides, and also important insights into the development of highly reversible metal borohydrides for hydrogen storage applications.
Zhang, XL, Zhang, X, Zhang, LC, Huang, ZG, Fang, F, Hu, JJ, Yang, YX, Gao, MX, Pan, HG & Liu, YF 2022, 'Ultrafast hydrogenation of magnesium enabled by tetragonal ZrO2 hierarchical nanoparticles', Materials Today Nano, vol. 18, pp. 100200-100200.
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Transition metal catalysts are particularly effective in improving the reaction kinetics of light metal hydrides for reversible hydrogen storage. Herein, tetragonal ZrO2 hierarchical nanoparticles (nano-ZrO2) composed of primary particles of ∼4 nm in diameter are successfully synthesized by a facile one-pot solvothermal process. The unique hierarchical structure features homogeneous distributions of in situ formed multivalent Zr-based species, which allow superior catalytic activity for hydrogen storage in MgH2. The MgH2+10 wt% nano-ZrO2 starts releasing H2 at 163 °C after one activation, which is 107 °C lower than additive-free MgH2, and 50 °C lower than that of bulk ZrO2-doped MgH2. At 230 °C, 5.9 wt% of H is rapidly liberated within 20 min from the nano-ZrO2-containing MgH2. More importantly, the material shows superior hydrogenation kinetics compared with all reported catalyst-modified MgH2. The nano-ZrO2-containing Mg took up 4.0 wt% of H in only 12 s at 100 °C under 50 bar H2, 400 times faster than the bulk-ZrO2-modified sample. Even at 50 °C, approximately 1.8 wt% H was absorbed within 1 min. Our findings provide useful insights into the design and development of high-performance catalysts toward solid-state hydrogen storage materials.
Zhang, Y, Chen, P, Wang, T, Su, D & Wang, C 2022, 'Development of Small‐Scale Monitoring and Modeling Strategies for Safe Lithium‐Ion Batteries', Batteries & Supercaps, vol. 5, no. 2.
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AbstractLithium‐ion batteries (LIBs) have the advantages of high energy density, stable working voltage, long cycling life, and no memory effect. They have been widely used as power sources for electric vehicles (EVs) and hybrid electric vehicles (HEVs). However, during periods of usage or storage, some unfavorable factors such as thermal runaway, volumetric expansion, and growth of lithium dendrites can severely reduce the reliability and safety of LIBs. Therefore, an accurate health estimation system and a reliable life expectancy strategy toward LIBs have been proved significantly important. However, due to the large volume and high price, most characterization methods in the laboratory cannot be applied directly to commercial electric devices. Therefore, small portable monitor methods are more practical. In this review, we first systematically reviewed the recent progress of modeling methods towards LIBs. Some typical modeling strategies (e. g., thermal models, electrical models and aging models) and advanced sensors which can be imbedded in LIBs are emphatically introduced and compared. At last, some promising directions of development on portable in‐situ monitor strategies are also predicted and supposed.
Zhang, Z, Yang, X, Li, P, Wang, Y, Zhao, X, Safaei, J, Tian, H, Zhou, D, Li, B, Kang, F & Wang, G 2022, 'Biomimetic Dendrite‐Free Multivalent Metal Batteries', Advanced Materials, vol. 34, no. 47, pp. e2206970-2206970.
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AbstractRechargeable multivalent metal (e.g., zinc (Zn) and aluminum (Al)) batteries are ideal choices for large‐scale energy storage owing to their intrinsic low cost and safety. However, the poor compatibility between metallic anodes and electrolytes strongly hampers their practical applications. Herein, it is demonstrated that confining multivalent metals in a biomimetic scaffold (Bio‐scaffold) can achieve highly efficient multivalent metal plating/stripping. This Bio‐scaffold is well‐tailored through the synergy of a parallel‐aligned array of fractal copper branches and a CaTiO3 (CTO)‐based coating layer. By virtue of this design strategy, the as‐developed Bio‐scaffold‐based Zn‐ and Al‐metal anodes exhibited dendrite‐free morphologies with high reversibility and long lifespan, as well as excellent performance for Zn and Al full batteries. Theoretical modeling and experimental investigations reveal that the fractal copper array not only facilitates multivalent ion diffusion and electrolyte wetting but also effectively reduces the local current densities during cycling; Meanwhile, the CTO‐based coating layer effectively blocks interfacial side reactions and enables a homogeneous ionic flux. This work opens a new avenue for developing multivalent metal batteries.
Zhao, S, Liu, Z, Xie, G, Guo, Z, Wang, S, Zhou, J, Xie, X, Sun, B, Guo, S & Wang, G 2022, 'High-efficiency cathode potassium compensation and interfacial stability improvement enabled by dipotassium squarate for potassium-ion batteries', Energy & Environmental Science, vol. 15, no. 7, pp. 3015-3023.
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A low-cost and high-efficiency K2C4O4 is used as a potassium reservoir source to boost the electrochemical performance of potassium-ion batteries, and how this strategy is expected to promote their practical application.
Zhou, F, Li, S, Ouyang, L, Liu, J, Liu, J, Huang, Z & Zhu, M 2022, 'Facile synthesis of black phosphorene via a low melting media assisted ball milling', Chemical Engineering Journal, vol. 444, pp. 136593-136593.
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Few-layer phosphorene (FLP) has attracted strong research interest due to its extraordinary physical and chemical properties. However, an efficient and rapid fabrication of high-quality FLP is still unavailable. Herein, a simple and efficient low melting media-assisted ball milling (LMMBM) approach is developed to prepare FLP in large quantities. The phase change of the LMM at higher temperatures leads to FLP with larger lateral dimensions compared to the ones obtained via dry solid state ball milling. Transmission electron microscope (TEM) studies indicated that liquid facilitates the slipping/curling of black phosphorus (BP) layers under the shearing force generated during ball milling. When used as an anode in Lithium-ion batteries, the FLP-C composite exhibits high initial Coulombic efficiency, stable cycling and rate capacity. This LMMBM approach can be adopted for mass production of other two-dimensional materials from their bulk counterparts.
Zhou, X, Wang, T, liu, H, Zhang, L, Zhang, C, Kong, N, Su, D & Wang, C 2022, 'Design of S-scheme heterojunction catalyst based on structural defects for photocatalytic oxidative desulfurization application', Journal of Photochemistry and Photobiology A: Chemistry, vol. 433, pp. 114162-114162.
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Carbon nitride (g-C3N4) is promising for many applications, but its photocatalytic activity is limited by weak visible light absorption and photogenerated carrier complexes. Herein, the thermally defective carbon nitride (d-C3N4) has a larger specific surface area and more reactive sites. d-C3N4 helped Ag3PO4 nanoparticles to be uniformly deposited on the surface of it and made it easier for particle dispersion. d-C3N4 and Ag3PO4 form an S-scheme heterojunction, facilitating the transfer and separation of photogenerated electrons and holes, and possessing high redox ability, which results in improved photocatalytic performance. The experimental results showed that the conversion of 10: 1 Ag3PO4/d-C3N4 for photocatalytic oxidative desulfurization (PODS) under visible light was as high as 92.5 % at 3 h, mainly due to the S-scheme heterojunction further promoting the transfer and separation of photogenerated carriers, suppressing the fast complexation and improving the efficiency of photocatalysis. In addition, the conversion mechanism of PODS was demonstrated using radical capture test, electron paramagnetic resonance spectrometer (EPR), and gas chromatography-mass spectrometry (GC–MS). This study helps researchers to understand the S-scheme heterojunctions constructed based on defects and provides new ideas for the design and application of photocatalysts.
Zhou, X, Wang, T, Zhang, L, Che, S, Liu, H, Liu, S, Wang, C, Su, D & Teng, Z 2022, 'Highly efficient Ag2O/Na-g-C3N4 heterojunction for photocatalytic desulfurization of thiophene in fuel under ambient air conditions', Applied Catalysis B: Environmental, vol. 316, pp. 121614-121614.
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A composite photocatalyst of Ag2O and Na doped g-C3N4 (Ag2O/Na-CN) with high efficiency was investigated for photocatalytic oxidative desulfurization (PODS). The concentration and lifetime of carriers are increased with Na-CN. Under light conditions, it produces more charge carriers for the generation of radical species, such as superoxide radicals and holes. In addition, Na-CN and Ag2O form a p-n heterojunction, facilitating the transfer and separation of photogenerated electrons and holes, and increasing the concentration of holes on the valence band of Ag2O. The significantly improved charge separation alone with the higher carrier concentration of Ag2O/Na-CN makes the activation and oxidation of thiophene easier. Free radical capture experiments, electron paramagnetic resonance, and gas chromatography-mass spectrometry tests showed that holes, electrons, and superoxide radicals are the most critical active species in the PODS process, supporting the proposed PODS mechanism.
Zhu, Y, Shen, S, Ouyang, L, Liu, J, Wang, H, Huang, Z & Zhu, M 2022, 'Effective synthesis of magnesium borohydride via B-O to B-H bond conversion', Chemical Engineering Journal, vol. 432, pp. 134322-134322.
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Magnesium borohydride (Mg(BH4)2) is widely regarded as a promising hydrogen storage material due to its high capacity; however, it is still challenging to synthesize Mg(BH4)2 with low cost. Traditionally, Mg(BH4)2 has been mainly produced using other borohydride as the starting materials via exchange reactions. Herein, we report an economical method to synthesize Mg(BH4)2 by converting B-O bonds in widely available borates or boric acid to B-H. The borates or boric acid is ball-milled with MgH2 under ambient conditions to form Mg(BH4)2 with high yield (>80%). Mg(BH4)2 was also successfully generated by reacting low-cost Mg with boric acid. Compared with previous approaches, this method avoids expensive boron sources such as LiBH4, NaBH4, and B2H6, and does not require high pressure H2 gas and high temperatures, and therefore significantly reduces costs. This method could be an alternative to the current Mg(BH4)2 synthesis processes.
Zou, P, Liu, J, Huang, Z, Hu, R & Ouyang, L 2022, 'Phenylphosphonic acid as a grain-refinement additive for a stable lithium metal anode', Chemical Communications, vol. 58, no. 91, pp. 12724-12727.
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The increased overpotential due to the complexation between phenylphosphonic acid and Li ions can reduce the grain size, boost nucleation rates, and prevent the formation of Li dendrites.
