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Interfacial Zn2+-solvation regulator towards reversible and stable Zn anode

Journal of Energy Chemistry 2025年第1期100卷 684-692页

作者： Miao Zhou Xiongbin Luo Hang Li Shan Guo Zhuang Tong Xiaotao Zhou Xu Li Zhaohui Hou Shuquan Liang guozhao fang College of Mechanical Engineering Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials Hunan Institute of Science and Technology School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South University College of Materials and Metallurgy Guizhou University National Energy Metal Resources and New Materials Key Laboratory Central South University

Aqueous zinc-ion batteries （AZIBs） are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc （Zn） deposition and hydrogen ***,the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn2+-solvation and deposition behavior demand comprehensive *** molecules endowed with special functional groups （such as hydroxyl,carboxyl,etc.） have the potential to significantly optimize the solvation structure of Zn2+and regulate the interfacial electric double layer （EDL）.By increasing nucleation overpotential and decreasing interfacial free energy,these functional groups facilitate a lower critical nucleation radius,thereby forming an asymptotic nucleation model to promote uniform Zn ***,this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn （H-Zn） anode with a uniform and dense *** interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques,indicating that the H-Zn anode exhibits dendrite-free growth,no by-products,and weak hydrogen evolution,in sharp contrast to the bare ***,the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 ***,the H-Zn//NH4V4O10（NVO） full battery showcases exceptional cycle stability,retaining 95.04%capacity retention after 400 cycles at a large current density of 5 A *** study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.

关键词： Aqueous zinc-ion batteries Interfacial reaction Asymptotic nucleation model Reversible and stable Zn anode

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Perspectives in Electrochemical in situ Structural Reconstruction of Cathode Materials for Multivalent-ion Storage

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Energy & Environmental Materials 2023年第1期6卷 72-86页

作者： Jing Huang Xuefang Xie Kun Liu Shuquan Liang guozhao fang School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083China School of Materials Science and Engineering Central South UniversityChangsha 410083China Hunan Key Laboratory of Mineral Materials and Application Central South UniversityChangsha 410083China Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083China

Multivalent-ion(such as Zn^(2+),Mg^(2+),Al^(3+))batteries are considered as a prospective alternative for large-scale energy ***,the main problem of cathode materials for multivalent-ion batteries is the sluggish diffusion of multivalent *** cathode materials will self-adjust under electrochemical conditions to achieve the optimal state for multivalent-ion *** this review,the significant role of electrochemical in situ structural reconstruction of cathode materials is *** types,basic characteristics,and formation mechanisms of reconstructed phases have been systematically discussed and *** most important insight we pointed out is that the cathode materials with loose structures after in situ electrochemical activation are conducive to the reversible diffusion of multivalent ***,several crucial issues of electrochemical activation and reconstruction were further analyzed and *** challenges and future perspectives are presented in the final section.

关键词： cathode materials electrochemical activation in situ reconstruction multivalent-ion batteries

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Ultra-High Mass-Loading Cathode for Aqueous Zinc-Ion Battery Based on Graphene-Wrapped Aluminum Vanadate Nanobelts

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Nano-Micro Letters 2019年第4期11卷 215-226页

作者： Wenyu Zhang Shuquan Liang guozhao fang Yongqiang Yang Jiang Zhou School of Materials Science and Engineering Central South UniversityChangsha 410083HunanPeople’s Republic of China Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083HunanPeople’s Republic of China

Rechargeable aqueous zinc-ion batteries(AZIBs)have their unique advantages of cost efficiency,high safety,and environmental ***,challenges facing the cathode materials include whether they can remain chemically stable in aqueous electrolyte and provide a robust structure for the storage of Zn2+.Here,we report on H11Al2V6O23.2@graphene(HAVO@G)with exceptionally large layer spacing of(001)plane(13.36?).The graphene-wrapped structure can keep the structure stable during discharge/charge process,thereby promoting the inhibition of the dissolution of elements in the aqueous *** used as cathode for AZIBs,HAVO@G electrode delivers ideal rate performance(reversible capacity of 305.4,276.6,230.0,201.7,180.6 mAh g?1 at current densities between 1 and 10 A g?1).Remarkably,the electrode exhibits excellent and stable cycling stability even at a high loading mass of^15.7 mg cm?2,with an ideal reversible capacity of 131.7 mAh g?1 after 400 cycles at 2 A g?1.

关键词： Aluminum vanadate Graphene Cathode High mass loading Aqueous zinc-ion battery

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Fundamental Understanding and Effect of Anionic Chemistry in Zinc Batteries

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Energy & Environmental Materials 2022年第1期5卷 186-200页

作者： Yuxin Gao Zhexuan Liu Shan Guo Xinxin Cao guozhao fang Jiang Zhou Shuquan Liang School of Materials Science and Engineering Central South UniversityChangsha 410083China Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083China

With the merit of high capacity,high safety,and low cost,zinc-ion batteries(ZIBs)possess huge application potential in the domain of large-scale energy ***,due to the relatively narrow voltage window and large lattice distortion of cationic redox reaction,ZIBs tend to present low energy density,poor kinetics,and unstable cyclic *** chemistry seems to provide a novel strategy to solve these issues from different aspects,such as enhanced operating voltage,extra capacity contribution,and boosted reaction *** the significance of this theory and the lack of relevant literatures,herein,in-depth comprehension of anionic chemistry and its positive effects on zinc storage performance have been emphasized and *** review aims to present a full scope of anionic chemistry and furnish systematic cognition for rational design of advanced ZIBs with high energy ***,insightful analysis and perspectives based on the current research status also have been proposed,which may point out some scientific suggestions and directions for the future research.

关键词： anionic chemistry electrode modification electrolyte regulation high energy density zinc-ion batteries

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Towards establishing uniform metrics for evaluating the safety of lithium metal batteries

Advanced Powder Materials

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Advanced Powder Materials 2023年第4期2卷 134-145页

作者： Zequan Zhao Xiyao Zhao Yiming Zhou Siliang Liu guozhao fang Shuquan Liang School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South UniversityChangsha410083China School of Metallurgy and Environment Central South UniversityChangsha410083China School of Ecology and Environment Hainan UniversityHaikou570228China Department of Mechanical and Aerospace Engineering The Hong Kong University of Science and TechnologyHong Kong999077China

Lithium metal batteries(LMBs)with ultra-high theoretical energy densities are regarded as excellent candidates for the next energy storage ***,there are many factors can cause the temperature of LMBs to exceed a safe range and trigger thermal *** effort has been invested in designing safe components of batteries to realize the application of ***,most studies only focus on one single aspect since there is no uniform metrics for evaluating the safety of ***,this review comprehensively summarizes all the trigger factors of thermal runaway and proposes the complete safety metrics of LMBs.A comprehensive overview of the development of safe LMBs is provided to discuss the gap between studies and practical ***,the future directions of academic research are proposed according to the challenges existing in current studies.

关键词： Thermal runaway Battery safety Lithium metal anode Lithium metal battery

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Boosting high initial coulombic efficiency of hard carbon by in-situ electrochemical presodiation

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Journal of Energy Chemistry 2023年第2期77卷 310-316,I0008页

作者： Nannan Qin Yanyan Sun Chao Hu Sainan Liu Zhigao Luo Xinxin Cao Shuquan Liang guozhao fang School of Materials Science and Engineering Central South UniversityChangsha 410083HunanChina School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083HunanChina College of Chemistry Xiangtan UniversityXiangtan 411105HunanChina Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083HunanChina

Hard carbon(HC)is a promising anode material for sodium ion batteries(SIBs),whereas inferior initial coulombic efficiency(ICE)severely limits its practical *** the present work,we propose an in situ electrochemical presodiation approach to improve ICE by mixing sodium biphenyl(Na-Bp)dimethoxyethane(DME)solution with DME-based ether electrolyte.A solid electrolyte interface(SEI)could be formed beforehand on the HC electrode and Na^(+)was absorbed to nanopores and graphene stacks,compensating for the sodium loss and preventing electrolyte decomposition during the initial charge and discharge *** this way,the ICE of half-cells was increased to nearly 100%and that of full-cells from 45%to 96%with energy density from 132.9 to 230.5 W h kg^(-1).Our work provides an efficient and facile method for improving ICE,which can potentially promote the practical application of HCbased materials.

关键词： Hard carbon In situ presodiation Initial coulombic efficiency Solid electrolyte interface Sodium-ion batteries

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Progress and prospect of low-temperature zinc metal batteries

Advanced Powder Materials

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Advanced Powder Materials 2022年第2期1卷 27-40页

作者： Zhexuan Liu Xiongbin Luo Liping Qin guozhao fang Shuquan Liang School of Materials Science and Engineering Central South UniversityChangsha410083China College of Biological and Chemical Engineering Guangxi University of Science and TechnologyLiuzhou545006China Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha410083China

The commercial application of aqueous zinc metal batteries in the field of large-scale energy storage is still suffered from their low-temperature operation,in which the electrochemical behaviors of the electrolyte,electrode materials,and their interfaces will deteriorate at low ***,by considering the significance of this topic,an in-depth comprehensive and systematic summary of low-temperature zinc metal batteries(LTZMBs)with the main challenges and corresponding optimization strategies was ***,the promising perspectives have also been proposed,aiming to guide the scientific future development of LTZMBs.

关键词： Zinc metal batteries Low-temperature performances Hydrogen bond Ionic conductivity Diffusion kinetics

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Reconstructing interfacial manganese deposition for durable aqueous zinc-manganese batteries

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National Science Review 2023年第10期10卷 139-150页

作者： Yida Hu Zhexuan Liu Lanyan Li Shan Guo Xuefang Xie Zhigao Luo guozhao fang Shuquan Liang School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South University School of Science Hunan University of Technology and Business College of Physical Science and Technology Xinjiang University College of Chemistry Xiangtan University

Low-cost,high-satety,and broad-prospect aqueous zinc-manganese batteries(ZMBs) are limited by complex interracial *** solid-liquid interfacial state of the cathode dominates the Mn dissolution/deposition process of aqueous ZMBs,especially the important influence on the mass and charge transfer behavior of Zn2+and Mn2+.We proposed a quasi-eutectic electrolyte(QEE) that would stabilize the reversible behavior of interracial deposition and favorable interracial reaction kinetic of manganese-based cathodes in a long cycle process by optimizing mass and charge *** emphasize that the initial interfacial reaction energy barrier is not the main factor affecting cycling performance,and the good reaction kinetics induced by interfacial deposition during the cycling process is more conducive to the stable cycling of the battery,which has been confirmed by theoretical analysis,quartz crystal microbalance with dissipation monitoring,depth etching X-ray photon-electron spectroscopy,*** a result,the QEE electrolyte maintained a stable specific capacity of 250 mAh g-1at 0.5 A g-1after 350 cycles in zinc-manganese *** energy density retention rate of the ZMB with QEE increased by 174%compared to that of conventional aqueous ***,the multi-stacked soft-pack battery with a cathodic mass load of 54.4 mg maintained a stable specific capacity of 200 mAh g-1for 100 cycles,demonstrating its commercial *** work proves the feasibility of adapting lean-water QEE to the stable aqueous ZMBs.

关键词： quasi-eutectic electrolyte aqueous zinc −manganese batteries solid −liquid interfacial state mass transfer charge transfer

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Suppressing by-product via stratified adsorption effect to assist highly reversible zinc anode in aqueous electrolyte

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Journal of Energy Chemistry 2021年第4期30卷 549-556页

作者： Miao Zhou Shan Guo guozhao fang Hemeng Sun Xinxin Cao Jiang Zhou Anqiang Pan Shuquan Liang School of Materials Science and Engineering Central South UniversityChangsha 410083HunanChina Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083HunanChina

The development of promising zinc anodes mainly suffers from their low plating/stripping coulombic efficiencies when using aqueous electrolyte,which are mainly associated with the interfacial formation of irreversible *** is urgent to develop technologies that can solve this issue ***,we report an artificial Sc_(2)O_(3) protective film to construct a new class of interface for Zn *** density functional theory simulation and experimental results have proven that the interfacial side reaction was inhibited via a stratified adsorption effect between this artificial layer and Zn *** from this novel structure,the Sc_(2)O_(3)-coated Zn anode can run for more than 100 cycles without short circuit and exhibit low voltage hysteresis,and the coulombic efficiency increases by 1.2%.Importantly,it shows a good application prospect when matched with two of popular manganese-based and vanadium-based *** excellent electrochemical performance of the Sc_(2)O_(3)-coated Zn anode highlights the importance of rational design of anode materials and demonstrates a good way for developing high-performance Zn anodes with long lifespan and high efficiency.

关键词： Zn anode Artificial protective film Stratified adsorption Interfacial reaction Zn4SO4(OH)6·H2O by-products

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Conversion-type anode chemistry with interfacial compatibility toward Ah-level near-neutral high-voltage zinc ion batteries

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National Science Review 2024年第7期11卷 226-238页

作者： Shan Guo Liping Qin Jia Wu Zhexuan Liu Yuhao Huang Yiman Xie guozhao fang Shuquan Liang School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South University College of Biological and Chemical Engineering Guangxi University of Science and Technology Information and Network Center Central South University

High-voltage aqueous zinc ion batteries（AZIBs） with a high-safety near-neutral electrolyte is of great significance for practical sustainable application; however, they suffer from anode and electrode/electrolyte interfacial incompatibility. Herein, a conversion-type anode chemistry with a low anodic potential, which is guided by the Gibbs free energy change of conversion reaction, was designed for high-voltage near-neutral AZIBs. A reversible conversion reaction between ZnC2O4·2H2O particles and three-dimensional Zn metal networks well-matched in CH3COOLi-based electrolyte was revealed. This mechanism can be universally validated in the battery systems with sodium or iodine ions. More importantly, a cathodic crowded micellar electrolyte with a water confinement effect was proposed in which lies the core for the stability and reversibility of the cathode under an operating platform voltage beyond 2.0 V, obtaining a capacity retention of 95% after 100 cycles. Remarkably, the scientific and technological challenges from the coin cell to Ah-scale battery, sluggish kinetics of the solid-solid electrode reaction, capacity excitation under high loading of active material, and preparation complexities associated with large-area quasi-solid electrolytes,were explored, successfully achieving an 88% capacity retention under high loading of more than 20 mg cm-2and particularly a practical 1.1 Ah-level pouch cell. This work provides a path for designing low-cost, eco-friendly and high-voltage aqueous batteries.

关键词： zinc compound anode conversion reaction voltage regulation interfacial design pouch cell

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