Asmara, AP, Chen, H & Ung, AT 2023, 'Preventing Adipogenesis and Preserving Mitochondria and GLUT-4 Functions by Extracts and Isolated Compounds of Australian Acacia saligna', Molecules, vol. 28, no. 18, pp. 6677-6677.
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Acacia saligna’s secondary metabolites show promise in treating type 2 diabetes mellitus and its related conditions. We previously discovered that methanolic extracts, isolated flavonoids, and cyclitols effectively preserve mitochondria in 3T3-L1 adipocytes. In this current work, quantification of lipid droplet levels with Oil Red O assay showed a noticeable decrease in lipogenesis in 3T3-L1 cells. Methanolic leaf and bark extracts and isolated compounds, (−)-epicatechin 6 and myricitrin 8, reduced cellular lipid levels by 21.15% to 25.28%, respectively. mRNA levels of key regulators of mitochondrial biogenesis, such as adiponectin, PGC-1α, and mtTFA, were increased. Methanolic flower extract (FL-MeOH) and its chemical components, naringenin 1 and D-(+)-pinitol 5a, increased these gene levels from 10% to 29% at the higher dose. Our study found that FL-MeOH slightly reduced pro-inflammatory cytokines TNF-α and IL-6, attributed to two phytochemicals, naringenin-7-O-α-L-arabinofuranoside 2 and D-(+)-pinitol 5a. Western blot analysis also showed that adipocytes treated with MeOH extracts had higher GLUT-4 expression levels than untreated adipocytes. Overall, A. saligna extracts and their isolated compounds demonstrated anti-lipogenesis activity during 3T3-L1 cell differentiation, modulation of transcriptional levels of adiponectin, PGC-1α, and mtTFA, reducing TNF-α and IL-6 mRNA levels, promoting mitochondrial biogenesis, and enhancing GLUT-4 expression.
Asmara, AP, Prasansuklab, A, Chiabchalard, A, Chen, H & Ung, AT 2023, 'Antihyperglycemic Properties of Extracts and Isolated Compounds from Australian Acacia saligna on 3T3-L1 Adipocytes', Molecules, vol. 28, no. 10, pp. 4054-4054.
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Our early work indicated that methanolic extracts from the flowers, leaves, bark, and isolated compounds of Acacia saligna exhibited significant antioxidant activities in vitro. The overproduction of reactive oxygen species (ROS) in the mitochondria (mt-ROS) interfered with glucose uptake, metabolism, and its AMPK-dependent pathway, contributing to hyperglycemia and diabetes. This study aimed to screen the ability of these extracts and isolated compounds to attenuate the production of ROS and maintain mitochondrial function via the restoration of mitochondrial membrane potential (MMP) in 3T3-L1 adipocytes. Downstream effects were investigated via an immunoblot analysis of the AMPK signalling pathway and glucose uptake assays. All methanolic extracts effectively reduced cellular ROS and mt-ROS levels, restored the MMP, activated AMPK-α, and enhanced cellular glucose uptake. At 10 µM, (−)-epicatechin-6 (from methanolic leaf and bark extracts) markedly reduced ROS and mt-ROS levels by almost 30% and 50%, respectively, with an MMP potential ratio 2.2-fold higher compared to the vehicle control. (−)-Epicatechin 6 increased the phosphorylation of AMPK-α by 43%, with an 88% higher glucose uptake than the control. Other isolated compounds include naringenin 1, naringenin-7-O-α-L-arabinopyranoside 2, isosalipurposide 3, D-(+)-pinitol 5a, and (−)-pinitol 5b, which also performed relatively well across all assays. Australian A. saligna active extracts and compounds can reduce ROS oxidative stress, improve mitochondrial function, and enhance glucose uptake through AMPK-α activation in adipocytes, supporting its potential antidiabetic application.
Asmara, AP, Prasansuklab, A, Tencomnao, T & Ung, AT 2023, 'Identification of Phytochemicals in Bioactive Extracts of Acacia saligna Growing in Australia.', Molecules, vol. 28, no. 3, pp. 1028-1028.
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Acacia saligna growing in Australia has not been fully investigated for its bioactive phytochemicals. Sequential polarity-based extraction was employed to provide four different extracts from individual parts of A. saligna. Bioactive extracts were determined using in vitro antioxidant and yeast α-glucosidase inhibitory assays. Methanolic extracts from barks, leaves, and flowers are the most active and have no toxicity against 3T3-L1 adipocytes. Compound isolation of bioactive extracts provided us with ten compounds. Among them are two novel natural products; naringenin-7-O-α-L-arabinopyranoside 2 and (3S*,5S*)-3-hydroxy-5-(2-aminoethyl) dihydrofuran-2(3H)-one 9. D-(+)-pinitol 5a (from barks and flowers), (-)-pinitol 5b (exclusively from leaf), and 2,4-di-t-butylphenol 7 are known natural products and new to A. saligna. (-)-Epicatechin 6, quercitrin 4, and myricitrin 8 showed potent antioxidant activities consistently in DPPH and ABTS assays. (-)-Epicatechin 6 (IC50 = 63.58 μM),D-(+)-pinitol 5a (IC50 = 74.69 μM), and naringenin 1 (IC50 = 89.71 μM) are the strong inhibitors against the α-glucosidase enzyme. The presence of these compounds supports the activities exerted in our methanolic extracts. The presence of 2,4-di-t-butylphenol 7 may support the reported allelopathic and antifungal activities. The outcome of this study indicates the potential of Australian A. saligna as a rich source of bioactive compounds for drug discovery targeting type 2 diabetes.
Bai, L, Song, A, Wang, L, Lei, X, Zhang, T, Tian, H, Liu, H, Qin, X, Wang, G & Shao, G 2023, 'Enhancement of hydrogen desorption for electrocatalytic hydrogen evolution on nickel-coupled graphite carbon nitride catalysts', Ionics, vol. 29, no. 1, pp. 323-330.
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Bai, Z, Wang, Z, Li, R, Wu, Z, Feng, P, Zhao, L, Wang, T, Hou, W, Bai, Y, Wang, G & Sun, K 2023, 'Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion', Nano Letters, vol. 23, no. 11, pp. 4908-4915.
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Brockbals, L, Garrett-Rickman, S, Fu, S, Ueland, M, McNevin, D & Padula, MP 2023, 'Estimating the time of human decomposition based on skeletal muscle biopsy samples utilizing an untargeted LC–MS/MS-based proteomics approach', Analytical and Bioanalytical Chemistry, vol. 415, no. 22, pp. 5487-5498.
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AbstractAccurate estimation of the postmortem interval (PMI) is crucial in forensic medico-legal investigations to understand case circumstances (e.g. narrowing down list of missing persons or include/exclude suspects). Due to the complex decomposition chemistry, estimation of PMI remains challenging and currently often relies on the subjective visual assessment of gross morphological/taphonomic changes of a body during decomposition or entomological data. The aim of the current study was to investigate the human decomposition process up to 3 months after death and propose novel time-dependent biomarkers (peptide ratios) for the estimation of decomposition time. An untargeted liquid chromatography tandem mass spectrometry–based bottom-up proteomics workflow (ion mobility separated) was utilized to analyse skeletal muscle, collected repeatedly from nine body donors decomposing in an open eucalypt woodland environment in Australia. Additionally, general analytical considerations for large-scale proteomics studies for PMI determination are raised and discussed. Multiple peptide ratios (human origin) were successfully proposed (subgroups < 200 accumulated degree days (ADD), < 655 ADD and < 1535 ADD) as a first step towards generalised, objective biochemical estimation of decomposition time. Furthermore, peptide ratios for donor-specific intrinsic factors (sex and body mass) were found. Search of peptide data against a bacterial database did not yield any results most likely due to the low abundance of bacterial proteins within the collected human biopsy samples. For comprehensive time-dependent modelling, increased donor number would be necessary along with targeted confirmation of proposed peptides. Overall, the presented results provide valuable information that aid in the understanding and estimation of the human decomposition processes. Graphical Abstract
Chen, P, Ouyang, L, Lang, C, Zhong, H, Liu, J, Wang, H, Huang, Z & Zhu, M 2023, 'All-pH Hydrogen Evolution by Heterophase Molybdenum Carbides Prepared via Mechanochemical Synthesis', ACS Sustainable Chemistry & Engineering, vol. 11, no. 9, pp. 3585-3593.
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Ding, Y, Zhang, S, Li, J, Sun, Y, Yin, B, Li, H, Ma, Y, Wang, Z, Ge, H, Su, D & Ma, T 2023, 'Enhanced Elastic Migration of Magnesium Cations in alpha‐Manganese Dioxide Tunnels Locally Tuned by Aluminium Substitution', Advanced Functional Materials, vol. 33, no. 2, pp. 2210519-2210519.
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AbstractThe harsh conditions of large hydrated ion radius of Mg2+ cations and the strong electrostatic interaction with the host material put forward higher requirements for high‐performance aqueous magnesium ion (Mg2+) energy storage devices. Herein, substituted aluminium ions (Al3+) doped α‐MnO2 materials are prepared. The introduction of Al3+ cations adjust the local chemical environment inside the tunnel structure of α‐MnO2 and precisely regulates the diffusion behavior of inserted Mg2+ cations. The shortened oxygens’ distance and abundant oxygen defects result in a substantially enhanced elastic migration pattern of Mg2+ cations driven by strengthened electrostatic attraction, which brings the lower diffusion energy barrier, improved reaction kinetics, and adaptive volume expansion as evidenced by Climbing Image‐Nudged Elastic Band density function theory calculations coupled with experimental confirmation in X‐ray photoelectron spectroscopy, electron paramagnetic resonance, and galvanostatic intermittent titration technique. As a result, this rationally designed cathode exhibits a high reversible capacity of 197.02 mAh g‐1 at 0.1 A g‐1 and stable cycle performance of 2500 cycles with 82% retention. These parameters are among the best of Mg‐ion capacitors reported to date. This study offers a detailed insight into the local tunnel structure tunning effect and opens up a new path of modification for tunnel‐type structural materials.
Dong, H, Qi, S, Wang, L, Chen, X, Xiao, Y, Wang, Y, Sun, B, Wang, G & Chen, S 2023, 'Conductive Polymer Coated Layered Double Hydroxide as a Novel Sulfur Reservoir for Flexible Lithium‐Sulfur Batteries', Small, vol. 19, no. 30.
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AbstractLithium‐sulfur battery (LSB) is widely regarded as the most promising next‐generation energy storage system owing to its high theoretical capacity and low cost. However, the practical application of LSBs is mainly hampered by the low electronic conductivity of the sulfur cathode and the notorious “shuttle effect”, which lead to high voltage polarization, severe over‐charge behavior, and rapid capacity decay. To address these issues, a novel sulfur reservoir is synthesized by coating polypyrrole (PPy) thin film on hollow layered double hydroxide (LDH) (PPy@LDH). After compositing with sulfur, such PPy@LDH‐S cathode shows a multi‐functional effect to reserve lithium polysulfides (LiPSs). In addition, the unique architecture provides sufficient inner space to encapsulate the volume expansion and enhances the reaction kinetics of sulfur‐based redox chemistry. Theoretical calculations have illustrated that the PPy@LDH has shown stronger chemical adsorption capability for LiPSs than those of porous carbon and LDH, preventing the shuttling of LiPSs and enhancing the nucleation affinity of liquid‐solid conversion. As a result, the PPy@LDH‐S electrode delivers a stable cycling performance and a superior rate capability. Flexible battery has demonstrated this PPy@LDH‐S electrode can work properly with treatments of bending, folding, and even twisting, paving the way for wearable devices and flexible electronics.
Elrahoumi, R, Zhu, L, Wagner, E, Maudez, W, Benvenuti, G, Phillips, MR & Ton-That, C 2023, 'Doping-induced Ti3+ state and oxygen vacancies in TiO2: A single-chip combinatorial investigation', Materials Chemistry and Physics, vol. 308, pp. 128283-128283.
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Faisal, SN, Do, T-TN, Torzo, T, Leong, D, Pradeepkumar, A, Lin, C-T & Iacopi, F 2023, 'Noninvasive Sensors for Brain–Machine Interfaces Based on Micropatterned Epitaxial Graphene', ACS Applied Nano Materials, vol. 6, no. 7, pp. 5440-5447.
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Farahmandjou, M, Lai, W, Safaei, J, Wang, S, Huang, Z, Marlton, F, Ruan, J, Sun, B, Gao, H, Ostrikov, KK, Notten, PHL & Wang, G 2023, 'Boosting the Electrochemical Performance of Lithium‐Rich Cathodes by Oxygen Vacancy Engineering', Batteries & Supercaps, vol. 6, no. 7.
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AbstractThe challenges of voltage decay and irreversible oxygen release for lithium‐rich layered oxide cathode materials have hindered their commercial application despite their high energy density and low cost. Herein, a facile post‐annealing strategy is developed to pre‐introduce oxygen vacancies (OVs) into Li1.2Mn0.457Ni0.229Co0.114O2 cathode materials. The induced OVs modify the local Mn coordination environments, enhance structural stability, and suppress oxygen release. The modified cathode exhibits a discharge capacity of 224.1 mAh g−1 at 0.1 C after 100 cycles with 97.7 % capacity retention. Even at 2 C, excellent capacity retention of 93.3 % after 300 cycles can be achieved. In situ and ex situ X‐ray diffraction are used to elucidate the reaction mechanisms and crystal structure during cycling tests. Ex situ X‐ray photoelectron spectroscopy confirmed the suppressed oxygen release, enhanced oxygen vacancies and reduced cathode‐electrolyte interfacial layer after cycling for the post‐annealed cathode. Our results show that the presence of oxygen vacancies through thermal expansion diminishes the phase transitions in cathode materials during the heating process. These findings contribute to developing next‐generation Li‐ion batteries (LIBs) by oxygen vacancy engineering for new cathode materials with improved electrochemical performances.
Farahmandjou, M, Lai, W, Safaei, J, Wang, S, Huang, Z, Marlton, F, Ruan, J, Sun, B, Gao, H, Ostrikov, KK, Notten, PHL & Wang, G 2023, 'Cover Feature: Boosting the Electrochemical Performance of Lithium‐Rich Cathodes by Oxygen Vacancy Engineering (Batteries & Supercaps 7/2023)', Batteries & Supercaps, vol. 6, no. 7.
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Feng, Z, Zhu, R, Chen, F, Zhu, Y, Zhou, Y, Guan, P, Kuo, Y-C, Fan, J, Wan, T, Li, M, Han, Z, Su, D & Chu, D 2023, 'Recent advances in water-induced electricity generation based on 2D materials: A review', Journal of Materials Research, vol. 38, no. 7, pp. 1757-1779.
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Fiedler, S, Ton-That, C & Phillips, MR 2023, 'Defect-free ZnO nanorods with high angular distribution for enhanced excitonic emission', Journal of Materials Research, vol. 38, no. 8, pp. 2145-2155.
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AbstractLow-temperature hydrothermal growth has emerged as a popular method for the fabrication of ZnO nanorods (NRs), increasing the functionality and utility of ZnO-based devices. In this work, we study the influence of growth time, temperature and seed layer on the dimensions and angular distribution of ZnO NRs. High-quality NRs with a crisscrossed 60° angular distribution have been grown with a 20–60 nm diameter and 600 nm length. We show that, within the ideal range of growth parameters, the growth time and temperature have no controllable influence on NR diameter and length, while the deposition method and size of the pre-growth deposited ZnO seeds affects diameter and NR angular alignment. We demonstrate advantages of using crisscross-aligned NRs over planar ZnO for the enhancement of ZnO excitonic emission by optical coupling with gold nanoparticles. These results can be readily adapted for applications that involve surface coating-mediated enhancement of both light emission and injection. Graphical abstract
Gao, X, Yang, N, Feng, J, Liao, J, Hou, S, Ma, X, Su, D, Yu, X, Yang, Z, Safaei, J, Wang, D & Wang, G 2023, 'Defect and interface control on graphitic carbon nitrides/upconversion nanocrystals for enhanced solar hydrogen production', National Science Open, vol. 2, no. 2, pp. 20220037-20220037.
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Goulden, T, Bodachivskyi, I, Padula, MP & Williams, DBG 2023, 'Concentrated ionic liquids for proteomics: Caveat emptor!', International Journal of Biological Macromolecules, vol. 253, pp. 127438-127438.
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Guan, P, Min, J, Chen, F, Zhang, S, Hu, L, Ma, Z, Han, Z, Zhou, L, Jia, H, Liu, Y, Sharma, N, Su, D, Hart, JN, Wan, T & Chu, D 2023, 'Enhancing the Electrochemical Properties of Nickel-Rich Cathode by Surface Coating with Defect-Rich Strontium Titanate', ACS Applied Materials & Interfaces, vol. 15, no. 24, pp. 29308-29320.
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Guan, P, Min, J, Chen, F, Zhang, S, Zhu, Y, Liu, C, Hu, Y, Wan, T, Li, M, Liu, Y, Su, D, Hart, JN, Li, Z & Chu, D 2023, 'Dual-modification of Ni-rich cathode materials through strontium titanate coating and thermal treatment', Journal of Colloid and Interface Science, vol. 652, pp. 1184-1196.
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Han, C, Li, W, Li, W, Yang, L & Huang, Z 2023, 'CoFeNi based trifunctional electrocatalysts featuring in-situ formed heterostructure', Inorganic Chemistry Communications, vol. 149, pp. 110402-110402.
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All-in-one transition metal-based electrocatalysts with high activities towards different reactions in aqueous electrolytes are of critical importance as they can dramatically bring down the cost of relevant energy devices. Herein a facile and low-cost synthesis of CoFeNi nanoparticles encapsulated by an N-doped carbon layer has been developed by pyrolyzing Prussian blue (PB) precursors. The obtained catalyst features tri-catalytic activity towards OER, ORR, and HER reactions in alkaline and acidic condition, and show great potential as a catalyst for water splitting and anode material for Zinc-Air batteries. Moreover, compared with the single phase, the sample with the heterostructure composed of both fcc and bcc phases exhibited dramatic enhancement in multi-catalytic activity. The heterostructure originates from an in-situ phase separation induced by composition variation. This demonstrates the effectiveness of heterostructure engineering introduced by in-situ phase separation in boosting the multi-catalytic activity.
Han, N, Zhang, W, Guo, W, Pan, H, Jiang, B, Xing, L, Tian, H, Wang, G, Zhang, X & Fransaer, J 2023, 'Designing Oxide Catalysts for Oxygen Electrocatalysis: Insights from Mechanism to Application', Nano-Micro Letters, vol. 15, no. 1.
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AbstractThe electrochemical oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O2 to water (H2O) or from O2 to hydrogen peroxide (H2O2). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments (e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.
Huang, M, Cao, C, Liu, L, Wei, W, Zhu, Q-L & Huang, Z 2023, 'Controlled synthesis of MOF-derived hollow and yolk–shell nanocages for improved water oxidation and selective ethylene glycol reformation', eScience, vol. 3, no. 5, pp. 100118-100118.
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Delicately designed metal–organic framework (MOF)-derived nanostructured electrocatalysts are essential for improving the reaction kinetics of the oxygen evolution reaction and tuning the selectivity of small organic molecule oxidation reactions. Herein, novel oxalate-modified hollow CoFe-based layered double hydroxide nanocages (h-CoFe-LDH NCs) and yolk–shell ZIF@CoFe-LDH nanocages (ys-ZIF@CoFe-LDH NCs) are developed through an etching–doping reconstruction strategy from a Co-based MOF precursor (ZIF-67). The distinctive nanostructures, along with the incorporation of the secondary metal element and intercalated oxalate groups, enable h-CoFe-LDH NCs and ys-ZIF@CoFe-LDH NCs to expose more active sites with high intrinsic activity. The resultant h-CoFe-LDH NCs exhibit outstanding OER activity with an overpotential of only 278 mV to deliver a current density of 50 mA cm−2. Additionally, controlling the reconstruction degree enables the formation of ys-ZIF@CoFe-LDH NCs with a yolk–shell nanocage nanostructure, which show outstanding electrocatalytic performance for the selective ethylene glycol oxidation reaction (EGOR) toward formate, with a Faradaic efficiency of up to 91%. Consequently, a hybrid water electrolysis system integrating the EGOR and the hydrogen evolution reaction using Pt/C||ys-ZIF@CoFe-LDH NCs is explored for energy-saving hydrogen production, requiring a cell voltage 127 mV lower than water electrolysis to achieve a current density of 50 mA cm−2. This work demonstrates a feasible way to design advanced MOF-derived electrocatalysts toward enhanced electrocatalytic reactions.
Huang, M, Zhou, S, Ma, D-D, Wei, W, Zhu, Q-L & Huang, Z 2023, 'MOF-derived MoC-Fe heterojunctions encapsulated in N-doped carbon nanotubes for water splitting', Chemical Engineering Journal, vol. 473, pp. 145170-145170.
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Engineering the synergistic interfacial structures in nanostructured electrocatalysts is an effective yet challenging pursuit. Here we report porous nitrogen-doped carbon nanotubes (NCNTs) entrapping heterojunctions between carbide and transition metal nanoparticles (NPs) as excellent bifunctional catalyst for hydrogen and oxygen evolution reactions (HER and OER). Dual-phase MoC and Fe NPs confined in NCNTs (denoted as MoC-Fe@NCNTs) was fabricated by trapping [Fe(C2O4)3]3– into Zn/Mo-HZIF framework followed by pyrolysis. The resultant catalyst exhibited commendable bifunctional activities with small overpotentials at 50 mA cm−2 for the HER of 252 and OER of 304 mV, respectively. Theoretical calculations and experimental observation prove that the combination of Fe NPs generates synergistic heterointerfaces and improves OER activity of MoC, thus endowing outstanding bifunctional electrocatalytic performances. Moreover, the NCNTs, as the electronic communication amplifier, can facilitate electron transfer and inhibit the aggregation and corrosion of the active species. The controllable fabrication of MOF-derived heterostructures reported in this work provides a prospect for developing bifunctional MOF derivatives for water electrolysis.
Huang, Z, Jaumaux, P, Sun, B, Guo, X, Zhou, D, Shanmukaraj, D, Armand, M, Rojo, T & Wang, G 2023, 'High-Energy Room-Temperature Sodium–Sulfur and Sodium–Selenium Batteries for Sustainable Energy Storage', Electrochemical Energy Reviews, vol. 6, no. 1.
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AbstractRechargeable room-temperature sodium–sulfur (Na–S) and sodium–selenium (Na–Se) batteries are gaining extensive attention for potential large-scale energy storage applications owing to their low cost and high theoretical energy density. Optimization of electrode materials and investigation of mechanisms are essential to achieve high energy density and long-term cycling stability of Na–S(Se) batteries. Herein, we provide a comprehensive review of the recent progress in Na–S(Se) batteries. We elucidate the Na storage mechanisms and improvement strategies for battery performance. In particular, we discuss the advances in the development of battery components, including high-performance sulfur cathodes, optimized electrolytes, advanced Na metal anodes and modified separators. Combined with current research achievements, this review outlines remaining challenges and clear research directions for the future development of practical high-performance Na–S(Se) batteries. Graphic Abstract
Huang, Z, Wang, S, Guo, X, Safaei, J, Lei, Y, Lai, W, Zhang, X, Sun, B, Shanmukaraj, D, Armand, M, Rojo, T & Wang, G 2023, 'A Hierarchical Hybrid MXenes Interlayer with Triple Function for Room‐Temperature Sodium‐Sulfur Batteries', Advanced Materials Technologies, vol. 8, no. 14.
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AbstractRoom temperature sodium sulfur (RT Na‐S) batteries with high theoretical energy density and low cost have recently gained extensive attention for potential large‐scale energy storage applications. However, the shuttle effect of sodium polysulfides is still the main challenge that leads to poor cycling stability, which hinders the practical application of RT Na‐S batteries. Herein, a multifunctional hybrid MXene interlayer is designed to stabilize the cycling performance of RT Na‐S batteries. The hybrid MXene interlayer comprises a large‐sized Ti3C2Tx nanosheets inner layer followed by a small‐sized Mo2Ti2C3Tx nanoflake outer layer on the surface of the glass fiber (GF) separator. The large‐sized Ti3C2Tx nanosheet inner layer provides an effective physical block and chemical confinement for the soluble polysulfides. The small‐sized Mo2Ti2C3Tx outer layer offers an excellent polysulfide trapping capability and accelerates the reaction kinetics of polysulfide conversion, due to its superior electronic conductivity, large specific surface area, and Mo‐rich catalytic surfaces. As a result, RT Na‐S batteries with this hybrid MXene interlayer modified glass fiber separator deliver a stable cycling performance over 200 cycles at 1 C with an enhanced capacity retention of 71%. This unique structure design provides a novel strategy to develop 2D material‐based functional interlayer for high‐performance metal‐sulfur batteries.
Ikram, M, Ilyas, B, Haider, A, Haider, J, Ul‐Hamid, A, Shahzadi, A, Goumri‐Said, S, Kanoun, MB, Nabgan, W & Mahmood, A 2023, 'Fabrication of La‐Doped MoS2 Nanosheets with Tuned Bandgap for Dye Degradation and Antimicrobial Activities, Experimental and Computational Investigations', Advanced Materials Interfaces, vol. 10, no. 14.
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AbstractThe development of efficient catalysts with a large number of active sites, tunable bandgap, and large surface area has been very challenging. In addition, a significant bottleneck in the application of catalysts for water treatment is their dissolution under extreme conditions, such as highly acidic or highly alkaline conditions that lead to poor application of the reported materials in real‐world applications. In this study, the lanthanum (La)‐doped molybdenum disulfide (MoS2) nanosheets are reported for efficient breakdown of toxic pollutants from wastewater under a wide pH range from strongly alkaline to strongly acidic solutions. The La‐MoS2 nanosheets (NSs) are prepared by a facile hydrothermal approach using a two‐step methodology. A redshift is observed upon La doping, indicating that the bandgap is lowered after La doping in MoS2. The changes in bandgap and electronic structure are further investigated using the density functional theory (DFT), which reveal that doping of La introduces new states within the bandgap region, allowing for further induced energy transitions. The La‐MoS2, having a doping concentration of 2%, exhibits the highest catalytic activity against methylene blue (MB) in neutral, acidic, and alkaline solutions, as well as substantial inhibitory activity for bacterial strains such as Escherichia coli (E. coli). In summary, the modified catalyst provides a pathway to design highly efficient catalysts for all pH range water treatment as well as good activity against microbes.
Jaumaux, P, Wang, S, Zhao, S, Sun, B & Wang, G 2023, 'Electrolyte Solvation Structure Design for High Voltage Zinc‐Based Hybrid Batteries', ENERGY & ENVIRONMENTAL MATERIALS, vol. 6, no. 4.
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Zinc (Zn) metal anodes have enticed substantial curiosity for large‐scale energy storage owing to inherent safety, high specific and volumetric energy capacities of Zn metal anodes. However, the aqueous electrolyte traditionally employed in Zn batteries suffers severe decomposition due to the narrow voltage stability window. Herein, we introduce N‐methylformamide (NMF) as an organic solvent and modulate the solvation structure to obtain a stable organic/aqueous hybrid electrolyte for high‐voltage Zn batteries. NMF is not only extremely stable against Zn metal anodes but also reduces the free water molecule availability by creating numerous hydrogen bonds, thereby accommodating high‐voltage Zn‖LiMn2O4 batteries. The introduction of NMF prevented hydrogen evolution reaction and promoted the creation of an F‐rich solid electrolyte interphase, which in turn hampered dendrite growth on Zn anodes. The Zn‖LiMn2O4 full cells delivered a high average Coulombic efficiency of 99.7% over 400 cycles.
Kabir, MM, Akter, MM, Huang, Z, Tijing, L & Shon, HK 2023, 'Hydrogen production from water industries for a circular economy', Desalination, vol. 554, pp. 116448-116448.
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Katzmarek, DA, Mancini, A, Maier, SA & Iacopi, F 2023, 'Direct synthesis of nanopatterned epitaxial graphene on silicon carbide', Nanotechnology, vol. 34, no. 40, pp. 405302-405302.
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Abstract This article introduces a straightforward approach for the direct synthesis of transfer-free, nanopatterned epitaxial graphene on silicon carbide on silicon substrates. A catalytic alloy tailored to optimal SiC graphitization is pre-patterned with common lithography and lift-off techniques to form planar graphene structures on top of an unpatterned SiC layer. This method is compatible with both electron-beam lithography and UV-lithography, and graphene gratings down to at least ∼100 nm width/space can be realized at the wafer scale. The minimum pitch is limited by the flow of the metal catalyst during the liquid-phase graphitization process. We expect that the current pitch resolution could be further improved by optimizing the metal deposition method and lift-off process.
Katzmarek, DA, Yang, Y, Ghasemian, MB, Kalantar-Zadeh, K, Ziolkowski, RW & Iacopi, F 2023, 'Characteristics of Epitaxial Graphene on SiC/Si Substrates in the Radio Frequency Spectrum', IEEE Electron Device Letters, vol. 44, no. 2, pp. 297-300.
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Khan, K, Tareen, AK, Iqbal, M, Ye, Z, Xie, Z, Mahmood, A, Mahmood, N & Zhang, H 2023, 'Recent Progress in Emerging Novel MXenes Based Materials and their Fascinating Sensing Applications', Small, vol. 19, no. 19, pp. 2206147-2206147.
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AbstractEarly transition metals based 2D carbides, nitrides and carbonitrides nanomaterials are known as MXenes, a novel and extensive new class of 2D materials family. Since the first accidently synthesis based discovery of Ti3C2in 2011, more than 50 additional compositions have been experimentally reported, including at least eight distinct synthesis methods and also more than 100 stoichiometries are theoretically studied. Due to its distinctive surface chemistry, graphene like shape, metallic conductivity, high hydrophilicity, outstanding mechanical and thermal properties, redox capacity and affordable with mass‐produced nature, this diverse MXenes are of tremendous scientific and technological significance. In this review, first we'll come across the MXene based nanomaterials possible synthesis methods, their advantages, limitations and future suggestions, new chemistry related to their selected properties and potential sensing applications, which will help us to explain why this family is growing very fast as compared to other 2D families. Secondly, problems that help to further improve commercialization of the MXene nanomaterials based sensors are examined, and many advances in the commercializing of the MXene nanomaterials based sensors are proposed. At the end, we'll go through the current challenges, limitations and future suggestions.
Khodasevych, I, Wesemann, L, Roberts, A & Iacopi, F 2023, 'Tunable nonlocal metasurfaces based on graphene for analogue optical computation', Optical Materials Express, vol. 13, no. 5, pp. 1475-1475.
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Meta-optical devices have recently emerged as ultra-compact candidates for real-time computation in the spatial domain. The use of meta-optics for applications in image processing and wavefront sensing could enable an order of magnitude increase in processing speed and data throughput, while simultaneously drastically reducing the footprint of currently available solutions to enable miniaturisation. Most research to date has focused on static devices that can perform a single operation. Dynamically tunable devices, however, offer increased versatility. Here we propose graphene covered subwavelength silicon carbide gratings as electrically tunable optical computation and image processing devices at mid-infrared wavelengths.
Lei, X, Ma, Z, Bai, L, Wang, L, Ding, Y, Song, S, Song, A, Dong, H, Tian, H, Tian, H, Meng, X, Liu, H, Sun, B, Shao, G & Wang, G 2023, 'Porous ZnP matrix for long‐lifespan and dendrite‐free Zn metal anodes', Battery Energy, vol. 2, no. 6.
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AbstractThe reversibility of Zn plating/stripping during cycling is adversely affected by dendritic growth, electrochemical corrosion, surface passivation, and hydrogen generation on the Zn anodes for rechargeable aqueous zinc ion batteries (ZIBs). Herein, through an ordinary anodic etching process, a uniform porous ZnP matrix protective layer was created on the Zn foil (Zn@ZnP). The large and accessible specific surface area of the prepared Zn@ZnP can facilitate contact with the electrolyte, accelerating the migration and enhancing the desolvation of Zn2+, effectively enhancing the Zn deposition kinetics. According to studies from scanning electron microscopy (SEM) and multiscale optical microscopy, the Zn@ZnP electrode effectively inhibits the growth of dendrites with excellent Zn plating/stripping reversibility. In consequence, the symmetric cell with the Zn@ZnP electrodes displays a long‐term cycle life of over 1260 h at 10 mA cm−2. The full cell, consisting of Zn@ZnP anodes and MnO2‐based cathode, demonstrated a high discharge capacity of 145 mAh g−1 after cycling 500 times at the current density of 1000 mA g−1. A scalable method for designing a homogeneous anode protection layer enables dendrite‐free zinc metal anodes, paving the way for interface modification of other metal anodes.
Li, C, Tareen, AK, Khan, K, Long, J, Hussain, I, Khan, MF, Iqbal, M, Xie, Z, Zhang, Y, Mahmood, A, Mahmood, N, Ahmad, W & Zhang, H 2023, 'Highly efficient, remarkable sensor activity and energy storage properties of MXenes and borophene nanomaterials', Progress in Solid State Chemistry, vol. 70, pp. 100392-100392.
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Li, Q, Han, N, Chai, J, Zhang, W, Du, J, Tian, H, Liu, H, Wang, G & Tang, B 2023, 'Strategies to improve metal-organic frameworks and their derived oxides as lithium storage anode materials', Energy, vol. 282, pp. 128378-128378.
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Li, X, Wang, Y, Wu, J, Tong, L, Wang, S, Li, X, Li, C, Wang, M, Li, M, Fan, W, Chen, X, Chen, Q, Wang, G & Chen, Y 2023, 'Engineering contact curved interface with high-electronic-state active sites for high-performance potassium-ion batteries', Proceedings of the National Academy of Sciences, vol. 120, no. 52.
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Potassium-ion batteries (PIBs) have attracted ever-increasing interest due to the abundant potassium resources and low cost, which are considered a sustainable energy storage technology. However, the graphite anodes employed in PIBs suffer from low capacity and sluggish reaction kinetics caused by the large radius of potassium ions. Herein, we report nitrogen-doped, defect-rich hollow carbon nanospheres with contact curved interfaces (CCIs) on carbon nanotubes (CNTs), namely CCI-CNS/CNT, to boost both electron transfer and potassium-ion adsorption. Density functional theory calculations validate that engineering CCIs significantly augments the electronic state near the Fermi level, thus promoting electron transfer. In addition, the CCIs exhibit a pronounced affinity for potassium ions, promoting their adsorption and subsequently benefiting potassium storage. As a result, the rationally designed CCI-CNS/CNT anode shows remarkable cyclic stability and rate capability. This work provides a strategy for enhancing the potassium storage performance of carbonaceous materials through CCI engineering, which can be further extended to other battery systems.
Lin, J, Yun, K, Sun, Q, Xiang, P, Wu, L, Yang, S, Dun, J, Fu, S & Chen, H 2023, 'How to sample a seizure plant: the role of the visualization spatial distribution analysis of Lophophora williamsii as an example', Forensic Sciences Research, vol. 8, no. 2, pp. 140-151.
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Abstract Natural compounds in plants are often unevenly distributed, and determining the best sampling locations to obtain the most representative results is technically challenging. Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI) can provide the basis for formulating sampling guideline. For a succulent plant sample, ensuring the authenticity and in situ nature of the spatial distribution analysis results during MSI analysis also needs to be thoroughly considered. In this study, we developed a well-established and reliable MALDI-MSI method based on preservation methods, slice conditions, auxiliary matrices, and MALDI parameters to detect and visualize the spatial distribution of mescaline in situ in Lophophora williamsii. The MALDI-MSI results were validated using liquid chromatography–tandem mass spectrometry. Low-temperature storage at −80°C and drying of “bookmarks” were the appropriate storage methods for succulent plant samples and their flower samples, and cutting into 40 μm thick sections at −20°C using gelatin as the embedding medium is the appropriate sectioning method. The use of DCTB (trans-2-[3-(4-tert-butylphenyl)-2-methyl-2-propenylidene]malononitrile) as an auxiliary matrix and a laser intensity of 45 are favourable MALDI parameter conditions for mescaline analysis. The region of interest semi-quantitative analysis revealed that mescaline is concentrated in the epidermal tissues of L. williamsii as well as in the meristematic tissues of the crown. The study findings not only help to provide a basis for determining the best sampling locations for mescaline in L. williamsii, but they also provide a reference for the optimization of storage and preparation conditions for raw plant organs before MALDI detection. ...
Liu, L, Ba, X, Guo, Y, Lei, G, Sun, X & Zhu, J 2023, 'Improved Iron Loss Prediction Models for Interior PMSMs Considering Coupling Effects of Multiphysics Factors', IEEE Transactions on Transportation Electrification, vol. 9, no. 1, pp. 416-427.
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This paper presents improved iron loss analytical prediction models for interior permanent magnet synchronous motors (IPMSMs) used in electric vehicles. The effects of slotting harmonics, pulse-width modulation (PWM) carrier harmonics, temperature rise and mechanical stress are considered in the proposed models. Specifically, by investigating the stator flux density as piecewise linear with trapezoidal waveform, the iron losses in the teeth and yoke regions are calculated separately, considering the different magnetic field distributions and waveforms. To deliberate the PWM harmonic influence, a correction coefficient is added to the hysteresis loss models, while the eddy current loss models are updated by summing all the eddy current losses caused by the power supplying current harmonics. Moreover, the coupling interaction effects of magnetic, thermal, and stress fields on the empirical coefficients of hysteresis and eddy current losses are analyzed in detail and also implemented in the iron loss prediction process. The feasibility and superiority of the proposed models are verified by numerical and experimental case studies on an IPMSM prototype.
Liu, Y, Zhang, W, Zhang, X, Yang, L, Huang, Z, Fang, F, Sun, W, Gao, M & Pan, H 2023, 'Nanostructured light metal hydride: Fabrication strategies and hydrogen storage performance', Renewable and Sustainable Energy Reviews, vol. 184, pp. 113560-113560.
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Hydrogen can play an important role in the development of a sustainable energy system. However, storing hydrogen in a safe, efficient and economical manner remains a huge challenge. Light metal hydrides have attracted considerable attention for hydrogen storage owing to their high gravimetric and volumetric hydrogen densities. However, the strong covalent and/or ionic bonds between metal atoms and hydrogen result in slow kinetics, poor reversibility, and temperatures too high for dehydrogenation, hence delaying their practical large–scale applications. Considerable efforts have been toward tailoring the thermodynamic and kinetic properties of light metal hydride–based hydrogen storage materials for performance improvement, with the fabrication of nanoscale particles being a key and effective strategy. This review covers the preparation methods and hydrogen storage performance of nanostructured light metal hydrides. The physical and chemical properties and hydrogen storage behaviors of reversible light metal hydrides are first summarized, including MgH2, borohydrides, aluminum hydrides, amide–hydride systems, and hydride composites. The second section focuses on the research progress in nanostructuring for enhancing the reversible hydrogen storage properties of these hydrides. Finally, the main challenges and the future research prospects are discussed. The combination of nanostructuring and nanocatalysis can significantly enhance the performance of these hydrides and make them practical hydrogen carriers.
Ma, H, Hu, M, Zhang, C, Jia, J, Fu, S, Wei, Z & Yun, K 2023, 'HPLC-MS/MS determination and the postmortem distribution or postmortem redistribution of paraquat and its metabolites in four fatal intoxication cases', Forensic Science International, vol. 345, pp. 111606-111606.
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Ma, Z, Song, A, Liu, Z, Guo, Y, Yang, X, Li, Q, Fan, Y, Dai, L, Tian, H, Qin, X, Liu, H, Shao, G & Wang, G 2023, 'Nanoconfined Expansion Behavior of Hollow MnS@Carbon Anode with Extended Lithiation Cyclic Stability', Advanced Functional Materials, vol. 33, no. 28.
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AbstractThe construction of hollow nanostructure by compositing with carbonaceous materials is generally considered an effective strategy to mitigate the drastic volume expansion of transition metal sulfides (TMSs) with high theoretical specific capacity in the process of lithium storage. However, designing well‐controlled architectures with extended lithiation cyclic stability, and ease the expansion of the electroactive materials into the reserved hollow spaces still needs to be developed. Herein, using MnS as an example, the hollow double‐shell carbon‐coated TMSs architecture is designed to achieve the controllable operation of shell thickness to regulate interfacial stress. The functional architecture enables the high‐capacity MnS to reach reversible capacities and extended lithiation cycling stability at high current densities. In situ transmission electron microscopy, optical observation characterizations and finite elements are used to analyze the nanoconfined expansion behavior of hollow MnS@C anodes. The as‐designed hollow structure with a carbon shell thickness ≈12.5 nm can effectively restrict the drastic expansion of MnS nanoshell into inner voids with compressive stress. This study demonstrates a general strategy to design functional carbon coating metal sulfides with tailored interfacial stress.
Man, Y, Jaumaux, P, Xu, Y, Fei, Y, Mo, X, Wang, G & Zhou, X 2023, 'Research development on electrolytes for magnesium-ion batteries', Science Bulletin, vol. 68, no. 16, pp. 1819-1842.
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Mao, S, Feng, A, Zhang, S, Onggowarsito, C, Chen, Q, Su, D & Fu, Q 2023, 'Investigation of structure–property–application relationships of a hydrogel-based solar vapor generator', Journal of Materials Chemistry A, vol. 11, no. 42, pp. 23062-23070.
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We correlated the hydration ability of different hydrophilic groups to the varying performance of their corresponding hydrogels in solar vapor generation (SVG), establishing the relationships between the chemical structure, hydration property, and applications.
Matar, F, Shi, Y-L, Ling, FC-C, Salih, A, Irvine, CP, De Silva, S, Phillips, MR & Ton-That, C 2023, 'Bandgap narrowing and hole self-trapping reduction in Ga2O3 by Bi2O3 alloying', Journal of Alloys and Compounds, vol. 960, pp. 170983-170983.
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Muhammad, I, Ahmed, S, Cao, H, Mahmood, A & Wang, Y-G 2023, 'Three-Dimensional Silicene-Based Materials: A Universal Anode for Monovalent and Divalent Ion Batteries', The Journal of Physical Chemistry C, vol. 127, no. 2, pp. 1198-1208.
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Muhammad, I, Ahmed, S, Cao, H, Yao, Z, Khan, D, Mahmood, A, Hussain, T, Xiong, X-G, Ahuja, R & Wang, Y-G 2023, '3D porous sulfur-graphdiyne with splendid electrocatalytic and energy storage application', Materials Today Chemistry, vol. 34, pp. 101756-101756.
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Navidpour, AH, Hosseinzadeh, A, Zhou, JL & Huang, Z 2023, 'Progress in the application of surface engineering methods in immobilizing TiO2 and ZnO coatings for environmental photocatalysis', Catalysis Reviews, vol. 65, no. 3, pp. 822-873.
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Photocatalysis is widely used for the degradation of organic pollutants, with TiO2 and ZnO as the best candidates with unique properties. However, agglomeration and recycling are major challenges in practical photocatalysis applications. Advanced deposition processes can provide nanotubular or hierarchical structures that are more promising than suspended particles. More importantly, higher efficiency of photoelectrocatalysis than photocatalysis for the degradation of persistent organic pollutants including perfluorooctanoic acid (PFOA) necessitates catalyst immobilization. Photoelectrocatalysis exhibited remarkably higher efficiency (56.1%) than direct photolysis (15.1%), electrocatalysis (5.0%) and photocatalysis (18.1%) for PFOA degradation. This paper aims to review the progress in the application of anodizing and thermal spraying as two major industrial surface engineering processes to bridge the gap between laboratorial and practical photocatalysis technology. Overall, thermal spraying is considered as one of the most efficient methods for the deposition of TiO2 and ZnO photocatalytic films.
Pradeepkumar, A, Cheng, HH, Liu, KY, Gebert, M, Bhattacharyya, S, Fuhrer, MS & Iacopi, F 2023, 'Low-leakage epitaxial graphene field-effect transistors on cubic silicon carbide on silicon', Journal of Applied Physics, vol. 133, no. 17.
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Epitaxial graphene (EG) on cubic silicon carbide (3C-SiC) on silicon holds the promise of tunable nanoelectronic and nanophotonic devices, some uniquely unlocked by the graphene/cubic silicon carbide combination, directly integrated with the current well-established silicon technologies. Yet, the development of graphene field-effect devices based on the 3C-SiC/Si substrate system has been historically hindered by poor graphene quality and coverage, as well as substantial leakage issues of the heteroepitaxial system. We address these issues by growing EG on 3C-SiC on highly resistive silicon substrates using an alloy-mediated approach. In this work, we demonstrate a field-effect transistor based on EG/3C-SiC/Si with gate leakage current 6 orders of magnitude lower than the drain current at room temperature, which is a vast improvement on the current literature, opening the possibility for dynamically tunable nanoelectronic and nanophotonic devices on silicon at the wafer level.
Qu, J, Cao, X, Gao, L, Li, J, Li, L, Xie, Y, Zhao, Y, Zhang, J, Wu, M & Liu, H 2023, 'Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering', Nano-Micro Letters, vol. 15, no. 1.
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AbstractElectrochemical carbon dioxide reduction reaction (CO2RR) provides a promising way to convert CO2 to chemicals. The multicarbon (C2+) products, especially ethylene, are of great interest due to their versatile industrial applications. However, selectively reducing CO2 to ethylene is still challenging as the additional energy required for the C–C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding of the key steps and preferred reaction pathways/conditions, as well as rational design of novel catalysts for ethylene production have been regarded as promising approaches to achieving the highly efficient and selective CO2RR. In this review, we first illustrate the key steps for CO2RR to ethylene (e.g., CO2 adsorption/activation, formation of *CO intermediate, C–C coupling step), offering mechanistic understanding of CO2RR conversion to ethylene. Then the alternative reaction pathways and conditions for the formation of ethylene and competitive products (C1 and other C2+ products) are investigated, guiding the further design and development of preferred conditions for ethylene generation. Engineering strategies of Cu-based catalysts for CO2RR-ethylene are further summarized, and the correlations of reaction mechanism/pathways, engineering strategies and selectivity are elaborated. Finally, major challenges and perspectives in the research area of CO2RR are proposed for future development and practical applications.
Safaei, J, Gao, Y, Hosseinpour, M, Zhang, X, Sun, Y, Tang, X, Zhang, Z, Wang, S, Guo, X, Wang, Y, Chen, Z, Zhou, D, Kang, F, Jiang, L & Wang, G 2023, 'Vacancy Engineering for High-Efficiency Nanofluidic Osmotic Energy Generation', Journal of the American Chemical Society, vol. 145, no. 4, pp. 2669-2678.
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Salih, AK, Phillips, MR & Ton-That, C 2023, 'Enhanced solar-driven water splitting performance using oxygen vacancy rich ZnO photoanodes', Solar Energy Materials and Solar Cells, vol. 259, pp. 112436-112436.
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Song, A, Song, S, Duanmu, M, Tian, H, Liu, H, Qin, X, Shao, G & Wang, G 2023, 'Recent Progress of Non‐Noble Metallic Heterostructures for the Electrocatalytic Hydrogen Evolution', Small Science, vol. 3, no. 9.
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Developing energy production, storage, and conversion technologies based on sustainable or renewable energy is essential to address the energy and environmental crisis. Electrochemical water splitting is one of the most promising approaches to realize the production of green hydrogen. The design of catalytic materials with low cost, high activity, and long‐term stability and the exploration of specific reaction mechanisms are the key focus for the involved electrochemical hydrogen evolution reaction (HER). Recently, substantial efforts have been devoted to the rational design and synthesis of non‐noble metallic heterostructures with fascinating synergistic effects among different components. These heterostructured materials demonstrate comprehensive properties exceeding the estimations by the rule of mixtures and display high activity and long‐term stability in industrial conditions for HER. Herein, the reaction mechanism and key parameters for improving catalytic performance in the HER process are discussed in detail. The latest advances in heterostructures based on synthetic methods and electrocatalytic characteristics from experimental and computational perspectives are summarized according to the role of various components. Herein, insights are provided in this review into an in‐depth understanding of the heterostructures as HER electrocatalysts, and the opportunities and challenges to scale up future‐oriented developments are highlighted.
Song, P, Li, J, Zhang, Y, Tang, F, Wang, C, Su, D & Wang, T 2023, 'Design of double-shelled NiS-FeS@NC hollow nanocubes for high-performance sodium-ion batteries', Journal of Alloys and Compounds, vol. 950, pp. 169905-169905.
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Song, P, Yang, J, Wang, C, Wang, T, Gao, H, Wang, G & Li, J 2023, 'Interface Engineering of Fe7S8/FeS2 Heterostructure in situ Encapsulated into Nitrogen-Doped Carbon Nanotubes for High Power Sodium-Ion Batteries', Nano-Micro Letters, vol. 15, no. 1.
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AbstractHeterostructure engineering combined with carbonaceous materials shows great promise toward promoting sluggish kinetics, improving electronic conductivity, and mitigating the huge expansion of transition metal sulfide electrodes for high-performance sodium storage. Herein, the iron sulfide-based heterostructures in situ hybridized with nitrogen-doped carbon nanotubes (Fe7S8/FeS2/NCNT) have been prepared through a successive pyrolysis and sulfidation approach. The Fe7S8/FeS2/NCNT heterostructure delivered a high reversible capacity of 403.2 mAh g−1 up to 100 cycles at 1.0 A g−1 and superior rate capability (273.4 mAh g−1 at 20.0 A g−1) in ester-based electrolyte. Meanwhile, the electrodes also demonstrated long-term cycling stability (466.7 mAh g−1 after 1,000 cycles at 5.0 A g−1) and outstanding rate capability (536.5 mAh g−1 at 20.0 A g−1) in ether-based electrolyte. This outstanding performance could be mainly attributed to the fast sodium-ion diffusion kinetics, high capacitive contribution, and convenient interfacial dynamics in ether-based electrolyte.
Tian, H, Song, A, Zhang, P, Sun, K, Wang, J, Sun, B, Fan, Q, Shao, G, Chen, C, Liu, H, Li, Y & Wang, G 2023, 'High Durability of Fe–N–C Single‐Atom Catalysts with Carbon Vacancies toward the Oxygen Reduction Reaction in Alkaline Media', Advanced Materials, vol. 35, no. 14, pp. 2210714-2210714.
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AbstractSingle‐atom catalysts (SACs) have attracted extensive interest to catalyze the oxygen reduction reaction (ORR) in fuel cells and metal–air batteries. However, the development of SACs with high selectivity and long‐term stability is a great challenge. In this work, carbon vacancy modified Fe–N–C SACs (FeH–N–C) are practically designed and synthesized through microenvironment modulation, achieving high‐efficient utilization of active sites and optimization of electronic structures. The FeH–N–C catalyst exhibits a half‐wave potential (E1/2) of 0.91 V and sufficient durability of 100 000 voltage cycles with 29 mV E1/2 loss. Density functional theory (DFT) calculations confirm that the vacancies around metal–N4 sites can reduce the adsorption free energy of OH*, and hinder the dissolution of metal center, significantly enhancing the ORR kinetics and stability. Accordingly, FeH–N–C SACs presented a high‐power density and long‐term stability over 1200 h in rechargeable zinc–air batteries (ZABs). This work will not only guide for developing highly active and stable SACs through rational modulation of metal–N4 sites, but also provide an insight into the optimization of the electronic structure to boost electrocatalytical performances.
Ung, AT & Asmara, AP 2023, 'Bioactive Phytochemicals of Acacia saligna', Molecules, vol. 28, no. 11, pp. 4396-4396.
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Acacia saligna is native to Western Australia. It has become an introduced and fast-growing plant in other parts of the world due to its ability to adapt to drought, saline and alkaline soils, and hast growing environments. Studies on the bioactivities and phytochemicals of the plant extracts were conducted. However, comprehensive information that links those bioactivities to the identified compounds in the plant’s extracts is still lacking. Data gathered in this review revealed a rich chemical diversity of hydroxybenzoic acids, cinnamic acids, flavonoids, saponins, and pinitols in A. saligna growing in Egypt, Saudi Arabia, Tunisia, South Africa, and Australia. The variability in phytochemical composition and quantity could be attributed to plant parts, growing locations, extraction solvents, and analysis methods. Identified phytochemicals support observed biological activities such as antioxidant, antimicrobial, anticancer, α-glucosidase inhibition, and anti-inflammation in the extracts. The knowledge of chemical structures, biological activities, and possible mechanisms of action of the bioactive phytochemicals identified in A. saligna were discussed. In addition, the structure–activity relationships of dominant active compounds were examined to explain the bioactivities exerted by A. saligna extracts. The review provides valuable insights towards future research and the development of new therapeutics from this plant.
Wang, H, Ma, J & Zhu, J 2023, 'Identifying household EV models via weighted power recurrence graphs', Electric Power Systems Research, vol. 217, pp. 109121-109121.
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Wang, L, Wang, R, Zheng, Q, Yao, X, Zhang, C, Fu, S, Wei, Z, Yun, K & Guo, Z 2023, 'Simulating dynamic interaction between diazepam and ethanol targeting the GABAA receptor via in silico model', NeuroToxicology, vol. 95, pp. 136-143.
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Wang, T, Gu, W, Yu, L, Guo, X, Yang, J, Sun, X, Guan, J, Zhou, L, Wang, C, Yao, H, Zhang, X & Wang, G 2023, 'MXene: An efficient hemoperfusion sorbent for the removal of uremic toxins', Journal of Materiomics, vol. 9, no. 6, pp. 1129-1140.
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Wang, X, Han, C, Li, H, Su, P, Ta, N, Ma, Y, Huang, Z & Liu, J 2023, 'Fabrication of monodispersed B, N co-doped hierarchical porous carbon nanocages through confined etching to boost electrocatalytic oxygen reduction', Nano Research, vol. 16, no. 1, pp. 290-298.
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Dual heteroatom-doped carbons have attracted widespread research attention as catalysts in the field of energy storage and conversion due to their unique electronic structures and chemical tunability. In particular, boron and nitrogen co-doped carbon (B,N@C) has shown great potential for photo/electrocatalytic applications. However, more needs to be done for rational designing and regulating the structure of these materials to improve their catalytic performance. Herein, monodispersed hierarchical porous B,N@C nanocages were fabricated by pyrolyzing zeolite imidazole framework (ZIF) which was treated with ammonia borane or boric acid via an integrated double-solvent impregnation and nanocofined-etching method. The treated ZIF-8 provided an essential structural template to achieve B, N co-doped hierarchical structures with micro/meso/macro multimodal pore size distributions. The resultant B,N@C nanocages displayed high catalytic activities for electrochemical oxygen reduction reaction (ORR) in alkaline media, outperforming most carbon-based catalysts, particularly from the perspective of the half-wave potentials. Such high catalytic performance is due to the enhanced activity by the coexistence of B and N and the mass transfer promoted by the unique hierarchical porous structure. [Figure not available: see fulltext.].
Wang, X, Liu, T, Li, H, Han, C, Su, P, Ta, N, Jiang, SP, Kong, B, Liu, J & Huang, Z 2023, 'Balancing Mass Transfer and Active Sites to Improve Electrocatalytic Oxygen Reduction by B,N Codoped C Nanoreactors', Nano Letters, vol. 23, no. 11, pp. 4699-4707.
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Mass transfer is critical in catalytic processes, especially when the reactions are facilitated by nanostructured catalysts. Strong efforts have been devoted to improving the efficacy and quantity of active sites, but often, mass transfer has not been well studied. Herein, we demonstrate the importance of mass transfer in the electrocatalytic oxygen reduction reaction (ORR) by tailoring the pore sizes. Using a confined-etching strategy, we fabricate boron- and nitrogen-doped carbon (B,N@C) electrocatalysts featuring abundant active sites but different porous structures. The ORR performance of these catalysts is found to correlate with diffusion of the reactant. The optimized B,N@C with trimodal-porous structures feature enhanced O2 diffusion and better activity per heteroatomic site toward the ORR process. This work demonstrates the significance of the nanoarchitecture engineering of catalysts and sheds light on how to optimize structures featuring abundant active sites and enhanced mass transfer.
Wang, X, Ye, R, Duyar, MS, Price, CAH, Tian, H, Chen, Y, Ta, N, Liu, H & Liu, J 2023, 'Design of mesoporous ZnCoSiOx hollow nanoreactors with specific spatial distribution of metal species for selective CO2 hydrogenation', Nano Research, vol. 16, no. 4, pp. 5601-5609.
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In heterogeneous catalysis, the precise placement of active components to perform unique functions in cooperation with each other is a tremendous challenge. The migration of matter on micro/nano-scale caused by diffusion is a promising pathway for design of catalytic nanoreactors with precise active sites location and controllable microenvironment through compartmentalization and confinement effects. Herein, we report two categories of mesoporous ZnCoSiOx hollow nanoreactors with different metal distributions and microenvironment engineered by the diffusion behavior of metal species in confined nanospace. Double-shelled hollow structures with well-distributed metal species were obtained by adopting core@shell structured ZnCo-zeolitic imidazolate framework (ZIF)@SiO2 as a template and employing three stages of hydrothermal treatment including the decomposition of ZIF, diffusion of metal species into the silica shell, and Ostwald ripening. Additionally, the formation of yolk@shell structure with a collective (Zn-Co) metal oxide as the yolk was achieved by direct pyrolysis of ZnCo-ZIF@SiO2. In CO2 hydrogenation, ZnCoSiOx with double-shelled hollow structures and yolk@shell structures respectively afford CO and CH4 as main product, which is related with different dispersion and location of active sites in the two catalysts. This study provides an efficient method for the synthesis of catalytic nanoreactors on the basis of insights of the atomic diffusion in confined space at the mesoscale. [Figure not available: see fulltext.].
Xiao, J, Xiao, Y, Li, J, Gong, C, Nie, X, Gao, H, Sun, B, Liu, H & Wang, G 2023, 'Advanced nanoengineering strategies endow high‐performance layered transition‐metal oxide cathodes for sodium‐ion batteries', SmartMat, vol. 4, no. 5.
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AbstractConsidering the abundance and low price of sodium, sodium‐ion batteries (SIBs) have shown great potential as an alternative to existing lithium‐based batteries in large‐scale energy storage systems, including electric automobiles and smart grids. Cathode materials, which largely decide the cost and the electrochemical performance of the full SIBs, have been extensively studied. Among the reported cathodes, layered transition‐metal oxides (LTMOs) are regarded as the most extremely promising candidates for the commercial application of the SIBs owing to their high specific capacity, superior redox potential, and suitable scalable preparation. Nevertheless, irreversible structural evolution, sluggish kinetics, and water sensitivity are still the critical bottlenecks for their practical utilization. Nanoengineering may offer an opportunity to address the above issues by increasing reactivity, shortening diffusion pathways, and strengthening structural stability. Herein, a comprehensive summary of the modification strategies for LTMOs is presented, emphasizing optimizing the structure, restraining detrimental phase transition, and promoting diffusion kinetics. This review intends to facilitate an in‐depth understanding of structure–composition–property correlation and offer guidance to the further development of the LTMO cathodes for next‐generation energy storage systems.
Xie, Y, Chen, X, Sun, K, Zhang, J, Lai, W, Liu, H & Wang, G 2023, 'Direct Oxygen‐Oxygen Cleavage through Optimizing Interatomic Distances in Dual Single‐atom Electrocatalysts for Efficient Oxygen Reduction Reaction', Angewandte Chemie International Edition, vol. 62, no. 17.
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AbstractThe oxygen reduction reaction (ORR) on transition single‐atom catalysts (SACs) is sustainable in energy‐conversion devices. However, the atomically controllable fabrication of single‐atom sites and the sluggish kinetics of ORR have remained challenging. Here, we accelerate the kinetics of acid ORR through a direct O−O cleavage pathway through using a bi‐functional ligand‐assisted strategy to pre‐control the distance of hetero‐metal atoms. Concretely, the as‐synthesized Fe−Zn diatomic pairs on carbon substrates exhibited an outstanding ORR performance with the ultrahigh half‐wave potential of 0.86 V vs. RHE in acid electrolyte. Experimental evidence and density functional theory calculations confirmed that the Fe−Zn diatomic pairs with a specific distance range of around 3 Å, which is the key to their ultrahigh activity, average the interaction between hetero‐diatomic active sites and oxygen molecules. This work offers new insight into atomically controllable SACs synthesis and addresses the limitations of the ORR dissociative mechanism.
Xie, Y, Chen, X, Sun, K, Zhang, J, Lai, W, Liu, H & Wang, G 2023, 'Direct Oxygen‐Oxygen Cleavage through Optimizing Interatomic Distances in Dual Single‐atom Electrocatalysts for Efficient Oxygen Reduction Reaction', Angewandte Chemie, vol. 135, no. 17.
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AbstractThe oxygen reduction reaction (ORR) on transition single‐atom catalysts (SACs) is sustainable in energy‐conversion devices. However, the atomically controllable fabrication of single‐atom sites and the sluggish kinetics of ORR have remained challenging. Here, we accelerate the kinetics of acid ORR through a direct O−O cleavage pathway through using a bi‐functional ligand‐assisted strategy to pre‐control the distance of hetero‐metal atoms. Concretely, the as‐synthesized Fe−Zn diatomic pairs on carbon substrates exhibited an outstanding ORR performance with the ultrahigh half‐wave potential of 0.86 V vs. RHE in acid electrolyte. Experimental evidence and density functional theory calculations confirmed that the Fe−Zn diatomic pairs with a specific distance range of around 3 Å, which is the key to their ultrahigh activity, average the interaction between hetero‐diatomic active sites and oxygen molecules. This work offers new insight into atomically controllable SACs synthesis and addresses the limitations of the ORR dissociative mechanism.
Xu, G, Zhang, X, Sun, S, Zhou, Y, Liu, Y, Yang, H, Huang, Z, Fang, F, Sun, W, Hong, Z, Gao, M & Pan, H 2023, 'Synergized Tricomponent All‐Inorganics Solid Electrolyte for Highly Stable Solid‐State Li‐Ion Batteries', Advanced Science, vol. 10, no. 25.
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AbstractGarnet‐type oxide Li6.4La3Zr1.4Ta0.6O12 (LLZTO) features superior ionic conductivity and good stability toward lithium (Li) metal, but requires high‐temperature sintering (≈1200 °C) that induces high fabrication cost, poor mechanical processability, and high interface resistance. Here, a novel high‐performance tricomponent composite solid electrolyte (CSE) comprising LLZTO−4LiBH4/xLi3BN2H8 is reported, which is prepared by ball milling the LLZTO−4LiBH4 mixture followed by hand milling with Li3BN2H8. Green pellets fabricated by heating the cold‐pressed CSE powders at 120 °C offer ultrafast room‐temperature ionic conductivity (≈1.73 × 10−3 S cm−1 at 30 °C) and ultrahigh Li‐ion transference number (≈0.9999), which enable the Li|Li symmetrical cells to cycle over 1600 h at 30 °C with only 30 mV of overpotential. Moreover, the Li|CSE|TiS2 full cells deliver 201 mAh g−1 of capacity with long cyclability. These outstanding performances are due to the low open porosity in the electrolyte pellets as well as the high intrinsic ionic conductivity and easy deformability of Li3BN2H8.
Yan, G, Sun, X, Zhang, Y, Li, H, Huang, H, Jia, B, Su, D & Ma, T 2023, 'Metal-Free 2D/2D van der Waals Heterojunction Based on Covalent Organic Frameworks for Highly Efficient Solar Energy Catalysis', Nano-Micro Letters, vol. 15, no. 1.
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Abstract Covalent organic frameworks (COFs) have emerged as a kind of rising star materials in photocatalysis. However, their photocatalytic activities are restricted by the high photogenerated electron–hole pairs recombination rate. Herein, a novel metal-free 2D/2D van der Waals heterojunction, composed of a two-dimensional (2D) COF with ketoenamine linkage (TpPa-1-COF) and 2D defective hexagonal boron nitride (h-BN), is successfully constructed through in situ solvothermal method. Benefitting from the presence of VDW heterojunction, larger contact area and intimate electronic coupling can be formed between the interface of TpPa-1-COF and defective h-BN, which make contributions to promoting charge carriers separation. The introduced defects can also endow the h-BN with porous structure, thus providing more reactive sites. Moreover, the TpPa-1-COF will undergo a structural transformation after being integrated with defective h-BN, which can enlarge the gap between the conduction band position of the h-BN and TpPa-1-COF, and suppress electron backflow, corroborated by experimental and density functional theory calculations results. Accordingly, the resulting porous h-BN/TpPa-1-COF metal-free VDW heterojunction displays outstanding solar energy catalytic activity for water splitting without co-catalysts, and the H2 evolution rate can reach up to 3.15 mmol g−1 h−1, which is about 67 times greater than that of pristine TpPa-1-COF, also surpassing that of state-of-the-art metal-free-based photocatalysts reported to date. In particular, it is the first work for constructing COFs-based heterojunctions with the help of h-BN, which may pro...
Yang, J, Guo, X, Gao, H, Wang, T, Liu, Z, Yang, Q, Yao, H, Li, J, Wang, C & Wang, G 2023, 'A High‐Performance Alloy‐Based Anode Enabled by Surface and Interface Engineering for Wide‐Temperature Sodium‐Ion Batteries', Advanced Energy Materials, vol. 13, no. 29.
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AbstractAlloy‐based anodes have shown great potential to be applied in sodium‐ion batteries (SIBs) due to their high theoretical capacities, suitable working potential, and abundant earth reserves. However, their practical applications are severely impeded by large volume expansion, unstable solid‐electrolyte interfaces (SEI), and sluggish reaction kinetics during cycling. Herein, a surface engineering of tin nanorods via N‐doped carbon layers (Sn@NC) and an interface engineering strategy to improve the electrochemical performance in SIBs are reported. In particular, the authors demonstrate that uniform surface modification can effectively facilitate electron and sodium transport kinetics, confine alloy pulverization, and simultaneously synergize interactions with the ether‐based electrolyte to form a robust organic‐inorganic SEI. Moreover, it is discovered that the diethylene glycol dimethyl ether electrolyte with strong stability and an optimized Na+ solvation structure can co‐embed the carbon layer to achieve fast reaction kinetics. Consequently, Sn@NC anodes deliver extra‐long cycling stability of more than 10 000 cycles. The full cell of Na3V2(PO4)3║Sn@NC exhibits high energy density (215 Wh kg−1), excellent high‐rate capability (reaches 80% capacity in 2 min), and long cycle life over a wide temperature range of −20 to 50 °C.
Yang, J, Wang, T, Guo, X, Sheng, X, Li, J, Wang, C & Wang, G 2023, 'Flexible sodium-ion capacitors boosted by high electrochemically-reactive and structurally-stable Sb2S3 nanowire/Ti3C2Tx MXene film anodes', Nano Research, vol. 16, no. 4, pp. 5592-5600.
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Yang, J, Yin, B, Zhang, S, Sun, Y, Li, J, Su, D & Ma, T 2023, 'Macromolecules Promoting Robust Zinc Anode by Synergistic Coordination Effect and Charge Redistribution', Small, vol. 19, no. 45.
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AbstractZn dendrite formation is the main obstacle to commercializing aqueous zinc–ion batteries (ZIBs). α‐cyclodextrin (α‐CD) is proposed as an environmentally friendly macromolecule additive in the ZnSO4‐based electrolyte to obtain stable and reversible Zn anodes. The results show that α‐CD molecules’ unique 3D structure can effectively regulate the mass transfer of the electrolyte components and isolate the Zn anode from H2O molecules. The α‐CD provides abundant electrons to the Zn (002) crystallographic plane, which induces charge density redistribution. Such an effect relieves the reduction and aggregation of Zn2+ cations while protecting the Zn metal anode from water molecules. Finally, a small amount of α‐CD additive (0.01 M) can enhance the performance of Zn significantly in Zn||Cu cells (1980 cycles with 99.45% average CE) and Zn||Zn cells (8000 h ultra‐long cycle life). The excellent practical applicability was further verified in Zn||MnO2 cells.
Yang, X, Zhang, B, Tian, Y, Wang, Y, Fu, Z, Zhou, D, Liu, H, Kang, F, Li, B, Wang, C & Wang, G 2023, 'Electrolyte design principles for developing quasi-solid-state rechargeable halide-ion batteries', Nature Communications, vol. 14, no. 1, p. 925.
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AbstractRechargeable halide-ion batteries (HIBs) are good candidates for large-scale due to their appealing energy density, low cost, and dendrite-free features. However, state-of-the-art electrolytes limit the HIBs’ performance and cycle life. Here, via experimental measurements and modelling approach, we demonstrate that the dissolutions in the electrolyte of transition metal and elemental halogen from the positive electrode and discharge products from the negative electrode cause the HIBs failure. To circumvent these issues, we propose the combination of fluorinated low-polarity solvents with a gelation treatment to prevent dissolutions at the interphase, thus, improving the HIBs’ performance. Using this approach, we develop a quasi-solid-state Cl-ion-conducting gel polymer electrolyte. This electrolyte is tested in a single-layer pouch cell configuration with an iron oxychloride-based positive electrode and a lithium metal negative electrode at 25 °C and 125 mA g–1. The pouch delivers an initial discharge capacity of 210 mAh g–1and a discharge capacity retention of almost 80% after 100 cycles. We also report assembly and testing of fluoride-ion and bromide-ion cells using quasi-solid-state halide-ion-conducting gel polymer electrolyte.
Yang, Y, Zhang, X, Zhang, L, Zhang, W, Liu, H, Huang, Z, Yang, L, Gu, C, Sun, W, Gao, M, Liu, Y & Pan, H 2023, 'Recent advances in catalyst-modified Mg-based hydrogen storage materials', Journal of Materials Science & Technology, vol. 163, pp. 182-211.
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The storage of hydrogen in a compact, safe and cost-effective manner can be one of the key enabling technologies to power a more sustainable society. Magnesium hydride (MgH2) has attracted strong research interest as a hydrogen carrier because of its high gravimetric and volumetric hydrogen densities. However, the practical use of MgH2 for hydrogen storage has been limited due to high operation temperatures and sluggish kinetics. Catalysis is of crucial importance for the enhancement of hydrogen cycling kinetics of Mg/MgH2 and considerable work has been focused on designing, fabricating and optimizing catalysts. This review covers the recent advances in catalyzed Mg-based hydrogen storage materials. The fundamental properties and the syntheses of MgH2 as a hydrogen carrier are first briefly reviewed. After that, the general catalysis mechanisms and the catalysts developed for hydrogen storage in MgH2 are summarized in detail. Finally, the challenges and future research focus are discussed. Literature studies indicate that transition metals, rare-earth metals and their compounds are quite effective in catalyzing hydrogen storage in Mg/MgH2. Most metal-containing compounds were converted in situ to elemental metal or their magnesium alloys, and their particle sizes and dispersion affect their catalytic activity. The in-situ construction of catalyzed ultrasmall Mg/MgH2 nanostructures (< 10 nm in size) is believed to be the future research focus. These important insights will help with the design and development of high-performance catalysts for hydrogen storage in Mg/MgH2.
Yao, Y, Qu, X, Zhou, L, Liu, Y, Hong, Z, Wu, Y, Huang, Z, Hu, J, Gao, M & Pan, H 2023, 'Rational Design of Robust and Universal Aqueous Binders to Enable Highly Stable Cyclability of High‐Capacity Conversion and Alloy‐Type Anodes', ENERGY & ENVIRONMENTAL MATERIALS, vol. 6, no. 5.
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The development of high‐performance binders is a simple but effective approach to address the rapid capacity decay of high‐capacity anodes caused by large volume change upon lithiation/delithiation. Herein, we demonstrate a unique organic/inorganic hybrid binder system that enables an efficient in situ crosslinking of aqueous binders (e.g., sodium alginate (SA) and carboxymethyl cellulose (CMC)) by reacting with an inorganic crosslinker (sodium metaborate hydrate (SMH)) upon vacuum drying. The resultant 3D interconnected networks endow the binders with strong adhesion and outstanding self‐healing capability, which effectively improve the electrode integrity by preventing fracturing and exfoliation during cycling and facilitate Li+ ion transfer. SiO anodes fabricated from the commercial microsized powders with the SA/0.2SMH binder maintain 1470 mAh g−1 of specific capacity at 100 mA g−1 after 200 cycles, which is 5 times higher than that fabricated with SA binder alone (293 mAh g−1). Nearly, no capacity loss was observed over 500 cycles when limiting discharge capacity at 1500 mAh g−1. The new binders also dramatically improved the performance of Fe2O3, Fe3O4, NiO, and Si electrodes, indicating the excellent applicability. This finding represents a novel strategy in developing high‐performance aqueous binders and improves the prospect of using high‐capacity anode materials in Li‐ion batteries.
Zhang, C, Feng, J, Guo, X, Zhang, J, Zhang, W, Zhang, L, Song, J, Shao, G & Wang, G 2023, 'Blocking polysulfide by physical confinement and catalytic conversion of SiO2@MXene for Li–S battery', Applied Physics Letters, vol. 122, no. 19.
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Lithium–sulfur (Li–S) batteries have attracted increasing attention for next-generation energy storage systems with a high energy density and low cost. However, the practical applications have been plagued by the sluggish reaction kinetics and the shuttle effect of lithium polysulfides (LiPSs). Herein, core–shell SiO2@Ti3C2Tx MXene (SiO2@MX) hollow spheres are constructed as multifunctional catalysts to boost the performance of Li–S batteries. The dual-polar and dual-physical properties of SiO2 core and MXene shell provide multiple defense lines to the shuttle effect by chemical and physical confinement to LiPSs. Density functional theory calculations prove that Ti3C2Tx MXene and SiO2 enable the stronger trapping ability of LiPSs and the fast Li2S decomposition process. With this strategy, the robust SiO2@MX/S electrodes deliver superior electrochemical performances, including a high capacity of 1263 mAh g−1, and remarkable cycling stability with an ultralow capacity decay of 0.04% per cycle over 1000 cycles at 1 C. This work highlights the significance of core-shell dual-polar structural sulfur catalysts for practical application in advanced Li–S batteries.
Zhang, L, Zhang, X, Zhang, W, Huang, Z, Fang, F, Li, J, Yang, L, Gu, C, Sun, W, Gao, M, Pan, H & Liu, Y 2023, 'Nanoparticulate ZrNi: In Situ Disproportionation Effectively Enhances Hydrogen Cycling of MgH2', ACS Applied Materials & Interfaces, vol. 15, no. 34, pp. 40558-40568.
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High thermal stability and sluggish absorption/desorption kinetics are still important limitations for using magnesium hydride (MgH2) as a solid-state hydrogen storage medium. One of the most effective solutions in improving hydrogen storage properties of MgH2 is to introduce a suitable catalyst. Herein, a novel nanoparticulate ZrNi with 10-60 nm in size was successfully prepared by co-precipitation followed by a molten-salt reduction process. The 7 wt % nano-ZrNi-catalyzed MgH2 composite desorbs 6.1 wt % hydrogen starting from ∼178 °C after activation, lowered by 99 °C relative to the pristine MgH2 (∼277 °C). The dehydrided sample rapidly absorbs ∼5.5 wt % H2 when operating at 150 °C for 8 min. The remarkably improved hydrogen storage properties are reasonably ascribed to the in situ formation of ZrH2, ZrNi2, and Mg2NiH4 caused by the disproportionation reaction of nano-ZrNi during the first de-/hydrogenation cycle. These catalytic active species are uniformly dispersed in the MgH2 matrix, thus creating a multielement, multiphase, and multivalent environment, which not only largely favors the breaking and rebonding of H-H bonds and the transfer of electrons between H- and Mg2+ but also provides multiple hydrogen diffusion channels. These findings are of particularly scientific importance for the design and preparation of highly active catalysts for hydrogen storage in light-metal hydrides.
Zhang, X, Lin, Y, Zhang, L, Huang, Z, Yang, L, Li, Z, Yang, Y, Gao, M, Sun, W, Pan, H & Liu, Y 2023, 'Hydrogen-assisted one-pot synthesis of ultrasmall TiC nanoparticles enhancing hydrogen cycling of sodium alanate', Chemical Engineering Journal, vol. 462, pp. 142199-142199.
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Zhang, X, Zhang, X, Zhang, L, Huang, Z, Fang, F, Yang, Y, Gao, M, Pan, H & Liu, Y 2023, 'Remarkable low-temperature hydrogen cycling kinetics of Mg enabled by VH nanoparticles', Journal of Materials Science & Technology, vol. 144, pp. 168-177.
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Nanoscaled catalysts have attracted much more attention due to their more abundant active sites and better dispersion than their bulky counterparts. In this work, VHx nanoparticles smaller than 10 nm in average size are successfully synthesized by a simple solid-state ball milling coupled with THF washing process, which are proved to be highly effective in enhancing the hydrogen absorption/desorption kinetics of MgH2 at moderate temperatures. The nano-VHx-modified MgH2 releases hydrogen from 182 °C, which is 88 °C lower than additive-free MgH2. The release of hydrogen amounts to 6.3 wt% H within 10 min at 230 °C and 5.6 wt% H after 30 min at 215 °C with initial vacuum. More importantly, the dehydrogenated MgH2+10 wt.% nano-VHx rapidly absorbs 5.2 wt% H within 3 min at 50 °C under 50 bar H2. It even takes up 4.3 wt% H within 30 min at room temperature (25 °C) under 10 bar H2, exhibiting superior hydrogenation kinetics to most of the previous reports. Mechanistic analyzes disclose the reversible transformation between V and V-H species during the hydrogen desorption-absorption process. The homogeneously distributed V-based species is believed to act as hydrogen pump and nucleation sites for MgH2 and Mg, respectively, thus triggering fast hydrogenation/dehydrogenation kinetics.
Zhang, X, Zhang, X, Zhang, L, Huang, Z, Yang, L, Gao, M, Gu, C, Sun, W, Pan, H & Liu, Y 2023, 'Nb2O5 Nanostructures as Precursors of Cycling Catalysts for Hydrogen Storage in MgH2', ACS Applied Nano Materials, vol. 6, no. 15, pp. 14527-14539.
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High operating temperatures and sluggish kinetics are major obstacles for practical applications of MgH2 as a solid hydrogen carrier. Introducing nanoscaled high-activity catalysts has been effective in improving the hydrogen cycling of MgH2. However, it remains still unclear that between nanoparticle size and morphology, which one is the decisive factor of the catalytic activity of a given catalyst. In this work, we studied this topic by taking nanostructured niobium oxide (Nb2O5) as a representative sample. Five types of Nb2O5 catalytic additives with different morphologies and nanosizes were synthesized, and their catalytic activities were compared with commercial microparticles. Our results unambiguously demonstrate that the catalytic activity of Nb2O5 is determined by the primary particle size rather than the morphology and structure because the ultrasmall Nb2O5 nanoparticles that measured ∼5 nm in size enable dehydrogenation of MgH2 starting at 165 °C after one-cycle activation. The smaller nanoparticle sizes not only enhance the reactivity of Nb2O5 but also lead to more uniform dispersion when ball-milled with MgH2, which enables in situ formation of more homogeneous and finer Nb-based active species and therefore much higher catalytic activity. This important insight will guide the design and optimization of novel high-activity catalysts for hydrogen cycling of MgH2 and other hydrogen storage materials.
Zhang, Y, Liu, H, Zhao, S, Xie, C, Huang, Z & Wang, S 2023, 'Insights into the Dynamic Evolution of Defects in Electrocatalysts', Advanced Materials, vol. 35, no. 9, pp. 2209680-2209680.
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AbstractThis review focuses on the formation and preparation of defects, the dynamic evolution process of defects, and the influence of defect dynamic evolution on catalytic reactions. The summary of the current advances in the dynamic evolution process of defects in oxygen evolution reaction, hydrogen evolution reaction, nitrogen reduction reaction, oxygen reduction reaction, and carbon dioxide reduction reaction, and the given perspectives are expected to provide a more comprehensive understanding of defective electrocatalysts on the structural evolution process during electrocatalysis and the reaction mechanisms, especially for the defect dynamic evolution on the performance in catalytic reactions.
Zhou, X, Liu, H, Liu, S, zhang, L, Wang, T, Wang, C & Su, D 2023, 'Constructing efficient ɑ-Fe2O3/g-C3N4/HNTs-loaded heterojunction photocatalysts for photocatalytic oxidative desulfurization: Influencing factors, kinetics, and mechanism', Fuel, vol. 332, pp. 126147-126147.
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The ɑ-Fe2O3/g-C3N4/HNTs (halloysite nanotubes) were prepared by a simple two-step calcination method. The HNTs skeleton increases the specific surface area of the material and enriches the adsorption reaction sites to prevent the reunion of g-C3N4, while ɑ-Fe2O3 further enhances the absorption in the visible region of g-C3N4. The transfer and separation of photogenerated carriers are promoted by the heterojunction structure constructed by ɑ-Fe2O3 and g-C3N4. The results showed that dibenzothiophene in model oil could be converted by 96.01 % in 3 h under visible light irradiation using ɑ-Fe2O3/g-C3N4/HNTs-10 as the photocatalyst. The electron paramagnetic resonance spectrometry, radical capture experiments, and gas chromatography-mass spectrometry indicated that hydroxyl radicals, holes, and superoxide radicals were the main active substances of the photocatalytic system. Based on the above experimental analysis, the photocatalytic desulfurization mechanism of ɑ-Fe2O3/g-C3N4/HNTs composites was proposed. This work opens a new path for the development of novel and advanced clay-based photocatalytic materials.
Zhu, Y, Li, J, Yang, L, Huang, Z, Yang, X-S, Zhou, Q, Tang, R, Shen, S & Ouyang, L 2023, 'Closed loops for hydrogen storage: Hydrolysis and regeneration of metal borohydrides', Journal of Power Sources, vol. 563, pp. 232833-232833.
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Zhu, Y, Zhu, R, Guan, P, Li, M, Wan, T, Hu, L, Zhang, S, Liu, C, Su, D, Liu, Y, Liu, D, Li, Q, Yu, J & Chu, D 2023, 'Designing MXene-Wrapped AgCl@Carbon core shell cathode for robust quasi-solid-state Ag-Zn battery with ultralong cycle life', Energy Storage Materials, vol. 60, pp. 102836-102836.
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