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Extended conjugation-induced π electron redistribution for stabilizing organic anodes in aqueous ammonium ion batteries

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Journal of Energy Storage 2025年 130卷

作者： Xinlei Tang Haode Zhang Sensen Yu Shan Hu Wen Chen State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 PR China

Organic molecules have attracted significant attention as potential anode materials for aqueous ammonium-ion batteries (AAIBs) due to their tunable structure, rich active sites, and abundant resources. However, their practical applications are hindered by structural instability and high solubility. Herein, we design an extended conjugated molecule, benzo[ a ]benzo[7,8]quinoxalino[2,3- i ]phenazine-8,17-dione (TABQ-NQ), by incorporating phenyl groups into the 5,7,12,14-tetraaza-6,13-pentacenequinone (TAPQ) structure. The strengthened intermolecular interactions arising from the extended conjugation contribute to the improved structural integrity of TABQ-NQ. Furthermore, the intramolecular charge redistribution facilitated by the extended conjugation enhances the binding affinity between TABQ-NQ and NH 4 + while reducing interactions of TABQ-NQ with H 2 O, thereby stabilizing discharge intermediates and preventing further dissolution. As a result, TABQ-NQ exhibits reduced solubility, improved stability, and superior electrochemical performance. The TABQ-NQ anode demonstrates a high initial specific capacity of 190 mAh g −1 , with a capacity of 146 mAh g −1 at 0.2 A g −1 after over 650 cycles, corresponding to the capacity retention of 76.8 %, and maintains an initial capacity of 127.5 mAh g −1 at 2 A g −1 . Ex-situ characterizations further reveal the low solubility and high redox reversibility of TABQ-NQ. This work provides new insights into the extension of conjugated structures in organic molecules and offers valuable guidance for the development of AAIBs research.

关键词： Aqueous ammonium-ion battery electron redistribution Extended π-conjugation Long-term stability Organic anode

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Controlling atomic phosphorous-mounting surfaces of ultrafine W_(2)C nanoislands monodispersed on the carbon frameworks for enhanced hydrogen evolution

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Chinese Journal of Catalysis 2021年第10期42卷 1798-1807页

作者： Xiangyong Zhang Tianying Liu Ting Guo Xueying Han Zongyun Mu Qiang Chen Jiangmin Jiang Jing Yan Jiaren Yuan Dezhi Wang Zhuangzhi Wu Zongkui Kou School of Materials Science and Engineering Central South UniversityChangsha 410083HunanChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina School of Physics and Electronic Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina

Controllably mounting foreign atoms on the surfaces of earth-abundant electrocatalysts strongly improve their surface electronic properties for optimizing the catalytic performance of surficial sites to an unusual level,and provides a good platform to gain deep insights into catalytic *** present work describes,employing ultrafine W2C nanoislands(average size:2.3 nm)monodispersed on the N,P dual-doped carbon frameworks as a model system,how to regulate the atomic phosphorous-mounting effect on the surfaces of W_(2)C to derive an active and stable P-mounting W_(2)C(WCP)catalyst for both acidic and alkaline hydrogen evolution reaction(HER).Since in situ phosphorus substitution into carbon sites of preformed W_(2)C nanoislands gradually proceeds from surfaces to solids,so that using a proper amount of phosphorus sources can readily control the surface mounting level to avoid the mass P-doping into the *** this way,the activity per active site of WCP catalyst with robust stability can be optimized to 0.07 and 0.56 H_(2 )s^(-1) at-200 mV overpotential in acid and base,respectively,which reach up to the several-fold of pure-phase W_(2)C(0.01 and 0.05 H_(2) s^(-1)).Theoretical investigations suggest that compared with solid P doping,the P mounting on W_(2)C surface can more remarkably enhance its metallicity and decrease the hydrogen release *** finding disclosed a key correlation between surface foreign atom-mounting and catalytic activity,and suggested a logical extension to other earth-abundant catalysts for various catalytic reactions.

关键词： Tungsten carbide Doping Surficial engineering Hydrogen evolution reaction Electrocatalyst

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ZnxCd1–xS quantum dot with enhanced photocatalytic H2-production performance

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Chinese Journal of Catalysis 2021年第1期42卷 15-24页

作者： Rongrong Gao Bei Cheng Jiajie Fan Jiaguo Yu Wingkei Ho State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina Department of Science and Environmental Studies The Education University of Hong KongHong KongChina

H2 is an important energy carrier for replacing fossil fuel in the future due to its high energy density and environmental *** a sustainable H2-generation method,photocatalytic H2 production by water splitting has attracted much ***,oil-soluble ZnxCd1-xS quantum dot(ZCS QD)with a uniform particle size distribution were prepared by a hot-injection ***,no photocatalytic H2-production activity was observed for the oil-soluble ZCS QD due to its ***,the oil-soluble ZCS QD was converted into a water-soluble ZCS QD by a ligand-exchange *** water-soluble ZCS QD exhibited excellent photocatalytic H2-production performance in the presence of glycerin and Ni^2+,with an apparent quantum efficiency of 15.9%under irradiation of 420 nm ***,the photocatalytic H2-generation activity of the ZCS QD was~10.7 times higher than that of the ZnxCd1-xS relative samples prepared by the conventional co-precipitation *** work will inspire the design and fabrication of other semiconductor QD photocatalysts because QD exhibits excellent separation efficiency for photogenerated electron-hole pairs due to its small crystallite size.

关键词： ZnxCd1-xS Solid-solution photocatalyst Photocatalytic H2 production Oil-soluble quantum dot Water-oil soluble quantum dot

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Novel N-Alkylation Synthetic Strategy of Imidazolium Cations Grafted Polybenzimidazole for High Temperature Proton Exchange Membrane Fuel Cells

SSRN

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SSRN 2022年

作者： Wang, Jian Liu, Guoliang Wang, Ailian Ji, Wenxi Zhang, Longgui Zhang, Taoyi Li, Jing Zhang, Hongfei Tang, Haolin Zhang, Haining State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Nr. 122 Luoshi Rd. Wuhan430070 China Foshan Xianhu Laboratory The Advanced Energy Science and Technology Guangdong Laboratory Foshan528200 China Research Institute of Chemical Industry Co. Ltd Beijing100013 China

Development of simple synthetic strategy of polybenzimidazole-based membranes with high uptake and retention ability of phosphoric acid is essential for long-term practical applications of high temperature proton exchange membrane fuel cells. In this work, N, N-dimethylacetamide is used as both deacid reagent and solvent for N-alkylation reaction to form imidazolium cations-grafted polybenzimidazole. The accordingly formed membranes exhibit an improved uptake and retention ability of phosphoric acid compared to pristine polybenzimidazole membrane. The optmized membrane with 60% of grafting degree has an acid uptake of 361.2 wt% with an anhydrous proton conductivity of 75.2 mS cm-1 at 160 oC, about 4.2 times higher than that of pristine polybenzimidazole membrane. After the acid retention test at 160 oC for 240 h, proton conductivity of the optimized membrane decreases by 7.5%, lower than that for pristine polybenzimidazole membrane under the same conditions (11.9% loss). The thus-assembled single cell delivers the power density of 0.430, 0.599 and 0.712 W cm-2 under 0, 100 and 200 kPa back pressures whereas the values are 0.321, 0.428 and 0.512 W cm-2 for the cell assembled from phosphoric acid-doped pristine polybenzimidazole membrane. © 2022, The Authors. All rights reserved.

关键词： Membranes

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Chemically Bonded Interface Construction of Covalent Organic Framework/CsPbBr3 Heterojunction for Efficient Photocatalytic CO2 Reduction Driven by Visible Light

SSRN

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SSRN 2024年

作者： Zhou, Min Wang, Zhiqing Mei, Aohan Chen, Keqiang Zeng, Jianrong Liu, Yueli Chen, Wen State Key Laboratory of Silicate Materials for Architectures School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China Sanya Science and Education Innovation Park Wuhan University of Technology Sanya572024 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China Faculty of Materials Science and Chemistry China University of Geosciences Wuhan430074 China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai201204 China

Effective interface interaction is the key factor to improve the photocatalytic performance due to its rapid interfacial charge transport. However, the complex organic synthesis environment and abundance surface ligands for most metal halide perovskites (MHPs) nanocrystals make it difficult to realize the strong interface interaction and rapid carrier transfer. Herein, the covalent organic framework (COF)/CsPbBr3 catalyst is constructed by in-situ growth method in HBr solvent. The Pb-N coordination acts as an electron delivery channel, guiding the transport of photogenerated carrier and enabling the effective separation of the photoexcited electron-hole pairs, thereby enhancing the performance of CO2 photoreduction. The photocatalytic efficiency of TpBpy/CsPbBr3 heterojunctions reaches up to 239.46 μmol·g–1 h–1 (CO) under the visible light irradiation, which is significantly higher than that of TpBpy and CsPbBr3 NCs. This work demonstrates a potential strategy for the construction of COF/MHPs heterojunction with strong interface interaction, which has great potential in various photocatalytic applications. © 2024, The Authors. All rights reserved.

关键词： Metal halides

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sp^(3)-like defect structure of hetero graphene-carbon nanotubes for promoting carrier transfer and stability

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Journal of Energy Chemistry 2021年第6期30卷 189-197,I0005页

作者： Shan-Shan Fan Ling Shen Yuan Dong Ge Tian Si-Ming Wu Gang-Gang Chang Christoph Janiak Ping Wei Jin-Song Wu Xiao-Yu Yang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing and School of Materials Science&EngineeringWuhan University of TechnologyWuhan 430070HubeiChina School of Chemistry Chemical Engineering and Life ScienceWuhan University of TechnologyWuhan 430070HubeiChina Institut für Anorganische Chemie und Strukturchemie Heinrich-Heine-Universität Düsseldorf40204 DüsseldorfGermany NRC(Nanostructure Research Centre) Wuhan University of TechnologyWuhan 430070HubeiChina Department of Engineering and Applied Sciences Harvard University CambridgeMA 02138United States

Three-dimensional(3 D) hybrid of nanocarbons is a very promising way to the high-performance design of electrocatalysis ***,sp^(3)-like defect structure,a combination of high strength and conduction of graphene and carbon nanotubes(CNTs) is rarely ***,3 D neural-like hybrids of graphene(from reduced graphene oxide) and carbon nanotubes(CNTs) have been integrated via sp^(3)-like defect structure by a hydrothermal *** sp^(3)-like defect structure endows 3 D nanocarbon hybrids with an enhanced carrier transfer,high structural stability,and electrocatalytic *** neural-like structure is shown to demonstrate a cascade effect of charges and significant performances regarding bio-electrocatalysis and lithium-sulfur energy *** concept and mechanism of "sp^(3)-like defect structure" are proposed at an atomic/nanoscale to clarify the generation of rational structure as well as the cascade electron transfer.

关键词： Graphene Carbon nanotubes sp^(3)-like defect structure Bio-electrocatalysis Lithium-sulfur batteries

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Influence of Substitution of Different Transition Metal Elements (Mn, Cr, Co) on the Properties of Bi0.88Sm0.12FeO3-Based Ceramics

SSRN

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SSRN 2022年

作者： Liu, Juan Wang, Le Jiang Zuo, Jia Nan Sun, Tu Lai Yu, Zi Long Xiang, Li Lin Guo, Xiang Tai Xu, Dong Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials School of Material Science and Engineering Anhui University of Technology Ma'anshan243002 China Center for Electron Microscopy State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology College of Chemical Engineering Zhejiang University of Technology Hangzhou310014 China

Transition metal elements (M=Mn, Cr, Co, Mn0.5Cr0.5, Mn0.5Co0.5, Cr0.5Co0.5) modified Bi0.88Sm0.12FeO3 (BSF-M) ceramics were synthesized by rapid liquid phase sintering. The effect of different transition metal elements on the structure and characteristics of BiFeO3-based ceramic were studied. Structural refinement revealed the coexistence of rhombohedral R3c phase, orthorhombic Pna21 phase and a small amount of Pbnm phase of all samples, and the element type had little effect on the phase composition. According to the XPS analysis, Co and Mn elements can be regarded as hard additives, and Cr element can be regarded as soft additives. Due to the different electronic structures of transition metal elements, different element substitutions have different effects on the electrical and magnetic properties of BiFeO3. The results show that the addition of Cr improved the electrical properties of BSF-based ceramics, and the best ferroelectric properties obtained in the BSF-Cr sample, where Pr =18.30 μC/cm2. The magnetic properties of Co substituted samples are significantly improved, and the maximum remanent magnetization obtained in the BSF-Co sample, where Mr =110.8 emu/mol, which may be attributed to the collinear magnetic structure induced by Co-substitution. Finally, the simultaneously enhanced ferroelectric and magnetic properties were obtained in the Cr and Co co-substituted composition BSF-Cr0.5Co0.5, where Pr =10.82 μC/cm2, Mr =73.3 emu/mol. Multiple ion substitution is a very effective method to optimize the properties of BiFeO3 © 2022, The Authors. All rights reserved.

关键词： Iron compounds

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Study of the Effect of Impregnation on Continuous Carbon Fibers Reinforced Sic Ceramic Composites Prepared Via material Extrusion and Reactive Melting Infiltration

SSRN

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SSRN 2022年

作者： Liu, Kai Qiu, Lei Zhang, Yuzhen Du, Yanying Sun, Ce Lu, Chao Zhang, Song Tu, Rong Wu, Yanjiao Sun, Huajun Shi, Yusheng State Key Laboratory of Silicate Materials for Architectures Wuhan University of Technology Wuhan430070 China School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China School of Logistics Engineering Wuhan University of Technology Wuhan430070 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Wuhan University of Technology China State Key Laboratory of Materials Processing and Die & Mould Technology Huazhong University of Science and Technology Wuhan430074 China

This paper presents a new method for the efficient preparation of continuous carbon fibers reinforced SiC ceramic (Cf/SiC) composites using material extrusion (MEX) and reactive melting infiltration (RMI). A slurry with the ability to produce stable filaments with good surface quality has been obtained by comparing the rheological behavior. The resin impregnation-carbonization and RMI processes were used for densification to obtain Cf/SiC composites. The effect of the number of impregnation-carbonization on the properties and microstructure of the sintered bodies has been studied. When the impregnation-carbonization was used for 1 time, the specific strength of the sintered body reached the highest value of 4.5 [[EQUATION]] 10 4 N·m/kg and the bending strength reached 93.1±4.3 MPa. In addition, Cf/SiC with complex structures were prepared using this method. This new approach reveals significant potential for MEX printing technology to prepare Cf/SiC composites with complex and lightweight structures. © 2022, The Authors. All rights reserved.

关键词： Carbon fibers

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Operando Observation of Structural Evolution and Kinetics of Li[Ni0.6Co0.2Mn0.2]O2 at Elevated Temperature

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Chemical Research in Chinese Universities 2020年第4期36卷 690-693页

作者： ZHANG Guobin PAN Xuelei YU Kesong YAN Mengyu XIONG Fangyu WU Liming DENG Xuanwci ZHANG Haining MAI Liqiang State Key Laboratory of Advanced Technology for Matehals Synthesis and Processing Wuhan University of TechnologyWuhan 430070P.R.China Department of Mechanical Engineering City University of Hong KongHong Kong 999077P.R.China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200P.R.China

Li[Ni0.6Co0.2Mn0.2]O2(NCM622)is one of the best commercialized cathodes in the battery ***,poor cyclability at relatively high temperature hinders its multiple ***,operando tests were performed to investigate the phase transitions and electron/ion transfer process of lavered NCM622 at 25 and 55℃.The identified spinel structure resulting in the poor cyclability at 55℃ guides the commercialization of batteries at high temperature.

关键词： Lithium-ion battery NCM622 High temperature In situ X-ray diffraction(XRD)

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Influence of Activation/Deactivation Process on Surface-Initiated Atom Transfer Radical Polymerization: An in Silico Investigation

SSRN

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SSRN 2024年

作者： Zhang, Zhongyan Li, Hui Guo, Yuqi Xue, Yao-Hong Liu, Hong Key Laboratory of Theoretical Chemistry of Environment Ministry of Education South China Normal University Guangzhou510006 China School of Chemistry South China Normal University Guangzhou510006 China State Key Laboratory of Advanced Processing and Recycling of Non-Ferrous Metal School of Material Science and Engineer Lanzhou University of Technology Lanzhou730050 China Department of Chemical and Material Engineering Lyuliang University Lishi033001 China Information Science School Guangdong University of Finance and Economics Guangzhou510320 China

We propose a simulation strategy to investigate the surface-initiated atom transfer radical polymerization (SI-ATRP), in which how the chain growth is affected by activation/deactivation process could be considered explicitly. We find the activation/deactivation process leads to that all polymer chains with equal opportunity of growth during SI-ATRP. The addition of more deactivator catalysts slows down the reaction process to induce more initiators, leading to the remarkable increase of grafting density, and meanwhile effectively yields decreased dispersity of grafted chains. The ratio of activated and dormant chains is theoretically proved to eventually reach equilibrated within the activation/deactivation process. The shorter lifetime of activation/deactivation cycle leads to an even equal opportunity and a faster "stop-continue" pace for the growth of all chains. Our study is helpful for better understanding the role of activation/deactivation process in SI-ATRP from a microscopic perspective, and also supplies the inspiration of better synthesizing polymer brushes with well-defined dispersity and grafting density. © 2024, The Authors. All rights reserved.

关键词： Molecular dynamics

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