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Biocompatible zinc battery with programmable electro-cross-linked electrolyte

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National Science Review 2023年第3期10卷 203-211页

作者： Xuesong Xie Jingjing Li Zhengyue Xing Bingan Lu Shuquan Liang Jiang Zhou School of Materials Science and Engineering Central South University Department of Plastic Surgery Xiangya Hospital of Central South University School of Physics and Electronics Hunan University

Aqueous zinc batteries(ZBs) attract increasing attention for potential applications in modern wearable and implantable devices due to their safety and stability.However,challenges associated with biosafety designs and the intrinsic electrochemistry of ZBs emerge when moving to practice,especially for biomedical devices.Here,we propose a green and programmable electro-cross-linking strategy to in situ prepare a multi-layer hierarchical Zn-alginate polymer electrolyte(Zn-Alg) via the superionic binds between the carboxylate groups and Zn2+.Consequently,the Zn-Alg electrolyte provides high reversibility of 99.6 5 %Coulombic efficiency(CE),>500 h of long-time stability and high bio compatibility(no damage to gastric and duodenal mucosa) in the body.A wire-shaped Zn/Zn-Alg/α-MnO2full battery affords 95% capacity retention after 100 cycles at 1 A g-1and good flexibility.The new strategy has three prominent advantages over the conventional methods:(ⅰ) the cross-linking process for the synthesis of electrolytes avoids the introduction of any chemical reagents or initiators;(ⅱ) a highly reversible Zn battery is easily provided from a micrometer to large scales through automatic programmable functions;and(ⅲ) high biocompatibility is capable of implanted and bio-integrated devices to ensure body safety.

关键词： polymer electrolyte green and programmable electro-cross-linking biocompatible zinc battery

Issues and Future Perspective on Zinc Metal Anode for Rechargeable Aqueous Zinc-ion Batteries

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Energy & Environmental Materials 2020年第2期3卷 146-159页

作者： Canpeng Li Xuesong Xie Shuquan Liang Jiang Zhou School of Materials Science and Engineering Central South UniversityChangsha Hunan 410083China Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Changsha Hunan 410083China

Rechargeable aqueous zinc-ion batteries(ZIBs) featuring the merits of low cost,eco-friendliness,and enhanced safety have attracted extensive interests and considered as the most promising energy storage system.However,much efforts are devoted to the exploration of cathode materials and their storage mechanisms in this system,and inadequate attentions are received in regard to anode side especially in neutral or mild acidic electrolyte.Therefore,in this review,the fundamental understanding of existing issues including dendrite formation,corrosion,and hydrogen evolution are mainly revealed,as well as their interaction in neutral or mild acidic medium.In addition,the currently existing solution strategies on the anode are summarized and the mechanisms that contained are simultaneously investigated.Finally,perspectives on future anode modification and innovation direction are provided for the further development and research of Zn-based ZIBs.

关键词： dendrite formation hydrogen evolution zinc corrosion zinc metal anode zinc-ion batteries

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 storage.However,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 performance.Anion 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 kinetics.Considering 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 summarized.This review aims to present a full scope of anionic chemistry and furnish systematic cognition for rational design of advanced ZIBs with high energy density.Furthermore,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

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 reactions.The 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 transfer.We 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,etc.As 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 batteries.The energy density retention rate of the ZMB with QEE increased by 174%compared to that of conventional aqueous electrolyte.Furthermore,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 potential.This 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

Integrated ‘all-in-one’ strategy to stabilize zinc anodes for high-performance zinc-ion batteries

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National Science Review 2022年第3期9卷 63-71页

作者： Canpeng Li Xuesong Xie Hui Liu Pinji Wang Canbin Deng Bingan Lu Jiang Zhou Shuquan Liang School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South University School of Physics and Electronics Hunan University

Many optimization strategies have been employed to stabilize zinc anodes of zinc-ion batteries(ZIBs).Although these commonly used strategies can improve anode performance, they simultaneously induce specific issues. In this study, through the combination of structural design, interface modification, and electrolyte optimization, an ’all-in-one’(AIO) electrode was developed. Compared to the three-dimensional(3D) anode in routine liquid electrolytes, the new AIO electrode can greatly suppress gas evolution and the occurrence of side reactions induced by active water molecules, while retaining the merits of a 3D anode. Moreover, the integrated AIO strategy achieves a sufficient electrode/electrolyte interface contact area, so that the electrode can promote electron/ion transfer, and ensure a fast and complete redox reaction. As a result, it achieves excellent shelving-restoring ability(60 hours, four times)and 1200 cycles of long-term stability without apparent polarization. When paired with two common cathode materials used in ZIBs(α-MnO2and NH4V4O10), full batteries with the AIO electrode demonstrate high capacity and good stability. The strategy of the ’all-in-one’ architectural design is enlightened to solve the issues of zinc anodes in advanced Zn-based batteries.

关键词： all-in-one electrode hydrogen-free electrode/electrolyte interface Zn-based batteries

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 application.In 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 cycle.By 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

Necklace-like Si@C nano?bers as robust anode materials for high performance lithium ion batteries

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Science Bulletin 2019年第4期64卷 261-269页

作者： Xiangzhong Kong Yuchao Zheng Yaping Wang Shuquan Liang Guozhong Cao Anqiang Pan School of Materials Science & Engineering Central South University Department of Materials Science & Engineering University of Washington Key Laboratory of Nonferrous Metal Materials and Engineering Ministry of Education Central South University

Silicon is believed to be a promising anode material for lithium ion batteries because of its highest theoretical capacity and low discharge potential. However, severe pulverization and capacity fading caused by huge volume change during cycling limits its practical application. In this work, necklace-like N-doped carbon wrapped mesoporous Si nanofibers(NL-Si@C) network has been synthesized via electrospinning method followed by magnesiothermic reduction reaction process to suppress these issues. The mesoporous Si nanospheres are wrapped with N-doped carbon shells network to form yolk-shell structure.Interestingly, the distance of adjacent Si@C nanospheres can be controllably adjusted by different addition amounts of SiO_2 nanospheres. When used as an anode material for lithium ion batteries, the NL-Si@C-0.5 exhibits best cycling stability and rate capability. The excellent electrochemical performances can be ascribed to the necklace-like network structure and N-doped carbon layers, which can ensure fast ions and electrons transportation, facilitate the electrolyte penetration and provide finite voids to allow large volume expansion of inner Si nanoparticles. Moreover, the protective carbon layers are also beneficial to the formation of stable solid electrolyte interface film.

关键词： Necklace-like Carbon shells network N-doped Mesoporous silicon Lithium ion batteries

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 storage.However,the main problem of cathode materials for multivalent-ion batteries is the sluggish diffusion of multivalent ions.Many cathode materials will self-adjust under electrochemical conditions to achieve the optimal state for multivalent-ion storage.In this review,the significant role of electrochemical in situ structural reconstruction of cathode materials is suggested.The types,basic characteristics,and formation mechanisms of reconstructed phases have been systematically discussed and commented.The 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 ions.Moreover,several crucial issues of electrochemical activation and reconstruction were further analyzed and discussed.The challenges and future perspectives are presented in the final section.

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

分级凝胶电解质调控Zn^(2+)配位隧道助力无枝晶锌负极

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Science Bulletin 2022年第9期67卷 955-962,M0004页

作者： Bingyao Zhang Liping Qin Yun Fang Yizhao Chai Xuesong Xie Bingan Lu Shuquan Liang Jiang Zhou School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South UniversityChangsha 410083China College of Biological and Chemical Engineering Guangxi University of Science and TechnologyLiuzhou 545006China School of Physics and Electronics Hunan UniversityChangsha 410083China

本文采用离子交联的方法,制备了高离子限域和氢键增强的单宁酸改性海藻酸基复合凝胶电解质.其中,单宁酸中的酚羟基和海藻酸钠中的羧基可以分别与锌离子进行配位和螯合,有效降低Zn^(2+)溶剂化壳层周围结合水分子的活性,通过增强的离子限... 详细信息

本文采用离子交联的方法,制备了高离子限域和氢键增强的单宁酸改性海藻酸基复合凝胶电解质.其中,单宁酸中的酚羟基和海藻酸钠中的羧基可以分别与锌离子进行配位和螯合,有效降低Zn^(2+)溶剂化壳层周围结合水分子的活性,通过增强的离子限域效应抑制了副反应和枝晶的生成,实现了锌的均匀沉积.利用该凝胶电解质组装的Zn/NH_(4)V_(4)O_(10)全电池搁置5d后,在2 A g^(-1)下循环200圈的容量保持率高达97.25%.同时,由于单宁酸中的羰基和海藻酸钠、水分子中的羟基之间形成强分子间氢键相互作用,电池在0℃低温下的循环稳定性也得到明显提升.此外,单宁酸中的酚羟基也可与钒基离子螯合,抑制循环过程中钒的溶解,为抑制钒基正极溶解和提高钒基电池小电流密度下的循环稳定性提供了新的解决方案.

关键词：凝胶电解质锌负极循环稳定性全电池单宁酸循环过程离子交联限域效应