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Lignin-reinforced PVDF electrolyte for dendrite-free quasi-solid-state Li metal battery

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Rare Metals 2024年第3期43卷 1006-1016页

作者： Xin-Yang Chen Xue-Jie Gao Han-Yan Wu Yu-Long Liu Xiao-Fei Yang Run-Cang Sun Center for Lignocellulosic Chemistry and Biomaterials College of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalian116034China Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China School of Chemistry Northeast Normal UniversityChangchun130024China

Quasi-solid-state lithium metal batteries(QSSLMBs)assembled with polyvinylidene fluoride(PVDF)are a promising class of next-generation rechargeable batteries due to their safety,high energy density,and superior interfacial properties.However,PVDF has a series of inherent drawbacks such as low ionic conductivity,ease of crystallization,and hydrophobic character that leading to poor cell properties.To tackle these issues,a lignin-reinforced PVDF electrolyte is proposed in this work to solve these drawbacks of PVDF and enhance the comprehensive performance of QSSBs.The lithophilic polar groups of lignin can promote uniform deposition of Li on the electrodes.Cooperating with the improved mechanical properties can efficiently prevent Li dendrites penetration through the separator.In addition,more active sites provided by lignin can also enhance Li^(+)transport and lead to a faster electrochemical reaction kinetic.Benefitting from the ingenious design,Li symmetric cells with 5%lignin-PVDF quasi-solid-state electrolyte can operate for 900 h at a high current density/capacity of 5 mA·cm^(-2)/5 mAh·cm^(-2),while shortcircuiting occurs after 56 h for the counterpart(pure PVDF).Moreover,a full cell of Li/5%lignin-PVDF/LFP cell demonstrates a high capacity of 96.2 mAh·g^(-1)after 2000 cycles at 10 C.This work is expected to open up promising opportunities to develop other high-energy/power-density QSSLMBs.

关键词： Quasi-solid-state electrolyte Lignin PVDF dendrite-free Li metal battery

dendrite-free Zn deposition initiated by nanoscale inorganic-organic coating-modified 3D host for stable Zn-ion battery

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SusMat 2024年第2期4卷 13-27页

作者： Jiaming Dong Junwen Duan Ruirui Cao Wang Zhang Kangkang Fang Hao Yang Ying Liu Zhitao Shen Fumin Li Rong Liu Mengqi Jin Longhui Lei Huilin Li Chong Chen Henan Key Laboratory of Photovoltaic Materials College of Future TechnologyHenan UniversityKaifengChina College of Optoelectronic Engineering Shenzhen UniversityShenzhenChina Institute of Solid-State Physics Chinese Academy of SciencesHefeiChina

A 3D nanostructured scaffold as the host for zinc enables effective inhibition of anodic dendrite growth.However,the increased electrode/electrolyte interface area provided by using 3D matrices exacerbates the passivation and localized corrosion of the Zn anode,ultimately bringing about the degradation of the electrochemical performance.Herein,a nanoscale coating of inorganic-organic hybrid(α-In_(2)Se_(3)-Nafion)onto a flexible carbon nanotubes(CNTs)framework(ISNF@CNTs)is designed as a Zn plating/stripping scaffold to ensure uniform Zn nucleation,thus achieving a dendrite-free and durable Zn anode.The intro-duced inorganic-organic interfacial layer is dense and sturdy,which hinders the direct exposure of deposited Zn to electrolytes and mitigates the side reactions.Meanwhile,the zincophilic nature of ISNF can largely reduce the nucleation energy barrier and promote the ion-diffusion transportation.Consequently,the ISNF@CNTs@Zn electrode exhibits a low-voltage hysteresis and a superior cycling life(over 1500 h),with dendrite-free Zn-plating behaviors in a typical symmetrical cell test.Additionally,the superior feature of ISNF@CNTs@Zn anode is further demonstrated by Zn-MnO_(2)cells in both coin and flexible quasi-solid-state configurations.This work puts forward an inspired remedy for advanced Zn-ion batteries.

关键词： 2D/3D configuration dendrite-free inorganic-organic layer interfacial protection Zn-ion batteries

Oxygen vacancies with localized electrons direct a functionalized separator toward dendrite-free and high loading LiFePO_(4)for lithium metal batteries

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Journal of Energy Chemistry 2022年第12期75卷 38-45,I0002页

作者： Qi An Qing Liu Shimin Wang Lixiang Liu Han Wang Yongjiang Sun Lingyan Duan Genfu Zhao Hong Guo School of Materials and Energy Yunnan UniversityNo.2Green Lake North RoadKunming 650091YunnanChina Institute for Integrative Nanosciences Leibniz IFW DresdenHelmholtzstraße 2001069 DresdenGermany

The pursuit of high energy density has promoted the development of high-performance lithium metal batteries(LMBs).However,the underestimated but non-negligible dendrites of Li anode have been observed to shorten battery lifespan.Herein,a composite separator(TiO_(2-x)@PP),in which TiO_(2)with electron-localized oxygen vacancies(TiO_(2-x))is coated on a commercial PP separator,is fabricated to homogenize lithium ion transport and stabilize the lithium anode interface.With the utilization of TiO_(2-x)@PP separators,the symmetric lithium metal battery displays enhanced cycle stability over 800 h under a high current density of 8 m A cm^(-2).Moreover,the LMBs assembled with high-loading LiFePO_(4)(9.24 mg cm^(-2))deliver a stable cycling performance over 900 cycles at a rate of 0.5 C.Comprehensive theoretical studies based on density functional theory(DFT)further unveil the mechanism.The favorable TiO_(2-x)is beneficial for facilitating fast Li+migration and impeding anions transfer.In addressing the Li dendrite issues,the use of TiO_(2-x)@PP separator potentially provides a facile and attractive strategy for designing well-performing LMBs,which are expected to meet the application requirements of rechargeable batteries.

关键词： Oxygen vacancy Ionic transport regulation dendrite-free Localized electrons High loading

Stabilizing zinc anode using zeolite imidazole framework functionalized separator for durable aqueous zinc-ion batteries

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Journal of Energy Chemistry 2024年第3期90卷 23-31,I0003页

作者： Weisong Zhang Xinyan Zhu Ling Kang Ziyu Peng Jing Zhu Liang Pan Lei Dai Shude Liu Ling Wang Yongguang Liu Zhangxing He School of Chemical Engineering North China University of Science and TechnologyTangshan 063009HebeiChina Shanghai Key Laboratory of Multidimensional Information Processing East China Normal UniversityShanghai 201620China College of Textiles Donghua UniversityShanghai 201620China

Aqueous zinc-ion batteries(AZIBs) hold great promise as a viable alternative to lithium-ion batteries owing to their high energy density and environmental friendliness.However,AZIBs are consistently plagued by the formation of zinc dendrites and concurrent side reactions,which significantly diminish their overall service life,In this study,the glass fiber separator(GF) is modified using zeolite imidazole salt framework-8(ZIF-8),enabling the development of efficient AZIBs.ZIF-8,which is abundant in nitrogen content,efficiently regulates the desolvation of [Zn(H_(2)O)_(6)]^(2+) to inhibit hydrogen production.Moreover,it possesses abundant nanochannels that facilitate the uniform deposition of Zn~(2+) via a localized action,thereby hindering the formation of dendrites.The insulating properties of ZIF-8 help prevent Zn^(2+) and water from trapping electron reduction at the layer surface,which reduces corrosion of the zinc anode.Consequently,ZIF-8-GF achieves the even transport of Zn^(2+) and regulates the homogeneous deposition along the Zn(002) crystal surface,thus significantly enhancing the electrochemical performance of the AZIBs,In particular,the Zn|Zn symmetric cell with the ZIF-8-GF separator delivers a stable cycle life at0.5 mA cm^(-2) of 2300 h.The Zn|ZIF-8-GF|MnO_(2) cell exhibits reduced voltage polarization while maintaining a capacity retention rate(93.4%) after 1200 cycles at 1.2 A g^(-1) The unique design of the modified diaphragm provides a new approach to realizing high-performance AZIBs.

关键词： Aqueous zinc-ion batteries Separators modifications ZIF-8 Zn deposition dendrite-free

Recent advances of ferro-/piezoelectric polarization effect for dendrite-free metal anodes

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稀有金属:英文版 2023年第8期42卷 2516-2544页

作者： Hai-Xia Zhang Peng-Fei Wang Chuan-Gang Yao Shi-Peng Chen Ke-Di Cai Fa-Nian Shi School of Materials Science and Engineering Shenyang University of TechnologyShenyang 110870China School of Environmental and Chemical Engineering Shenyang University of TechnologyShenyang 110870China College of Chemistry and Materials Engineering Bohai UniversityJinzhou 121013China

Metal anodes based on plating/stripping electrochemistry,for instance,common alkaline metal lithium(Li),sodium(Na),potassium(K),polyvalent metal magnesium(Mg),aluminum(Al),calcium(Ca)and zinc(Zn)are imminently evoked and increasingly researched for future generation high-energy-density rechargeable batteries due to their large theoretical capacity,low electrochemical potential,and superior electronic conductivity in recent years.However,the uncontrolled dendrite formation issue induces low Coulombic efficiency,short lifespan,and hazardous security risks,hindering the actual applications of metal batteries.Among various solutions,the utilization of ferro-/piezoelectric materials for metal anodes displays active effects on decreasing local current density,suppressing dendrite growth,and tolerating volume expansion benefits from the unique ferro-/piezoelectric polarization effect.This review presents the research progress of ferro-/piezoelectric polarization effect for regulating the dendritic growth of metal anodes for the first time.First,the current challenges and strategies of metal anodes are proposed.Then,ferro-/piezoelectric materials and their working principle are discussed.Finally,the recent research progress of ferroelectric and piezoelectric materials on dynamic regulation of dendrite growth is summarized,and the future perspectives are prospected.We hope this review could draw more attention in designing metal anodes with self-polarization materials and promoting their practical applications.

关键词： Metal anode Ferro-/piezoelectric material Polarization effect dendrite-free Lithium Perovskite

A Janus separator towards dendrite-free and stable zinc anodes for long-duration aqueous zinc ion batteries

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Journal of Energy Chemistry 2023年第6期81卷 583-592,I0013页

作者： Yan Sun Qinping Jian Tianshuai Wang Bin Liu Yuhan Wan Jing Sun Tianshou Zhao Department of Mechanical and Aerospace Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077China Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055GuangdongChina School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an 710129ShaanxiChina

Critical issues of Zn anodes including undesirable dendrites formation and parasitic reactions severely limit the reversibility and cyclability of Zn anodes.To address these issues,a functional Janus separator with the structure of a mechanically strong sulfonated poly(arylene ether sulfone)(SPAES)dense layer composited on a porous glass fiber(GF)substrate is designed.The SPAES dense layer that faces the Zn anode containing abundant sulfonic acid groups effectively promotes the desolvation process of hydrated Zn ions,guides uniform Zn ion transfer,and blocks anions and water,contributing to dendrite-free and highly reversible Zn plating/stripping cycles,while the porous GF substrate retains high electrolyte uptake.As a result,the Zn symmetric cell with the Janus separator demonstrates an ultralong cycling lifespan of over 2000 h at the areal capacity of 1 m A h cm^(-2),which is 23-fold superior to that with a pristine glass fiber separator(dendrites formation and ameliorating the parasitic reactions of Zn metal anodes for high-performance Zn ion batteries.

关键词： Janus separator Sulfonated poly(arylene ether sulfone) dendrite-free Side reaction suppression Aqueous zinc-ion batteries

The thermodynamically directed dendrite-free lithium metal batteries on LiZn alloy surface

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Nano Research 2023年第6期16卷 8354-8359页

作者： Huanqin Zheng Xu Cheng Quan Zheng Jianjun Zhang Tao Li Erqing Xie Ying Xu School of Physical Science and Technology Lanzhou UniversityLanzhou 730000China School of Materials and Energy Lanzhou UniversityLanzhou 730000China Southeast Research Institute of Lanzhou University Fujian 351100China

Metical lithium(Li)is one of the most promising alternatives as an anode in next-generation high energy batteries for its high theoretical specific capacity and low redox potential.However,severe Li dendrite growth leading to poor stability and safety issues hinders its practical implementation.Herein,three-dimensional carbon cloth(CC)with full zinc oxide quantum dots(ZnO QDs)covering is rationally chosen as the substrate for the suppression of Li dendrite.Owing to the spontaneous reaction between ZnO QDs and molten Li,LiZn alloy is formed and covered on CC,which endows substrate with high affinity for Li adsorption and suitable barrier energy for Li diffusion.This thermodynamic regulation on substrate is beneficial for homogeneous Li nucleation and deposition,thus enabling high stability for over 1,900 h at ultrahigh current density of 10 mA∙cm^(−2) in symmetrical cell and delivering superior performance in full batteries.

关键词： LiZn alloy adsorption energy diffusion barrier dendrite-free Li metal batteries

High-adhesion anionic copolymer as solid-state electrolyte for dendrite-free Zn-ion battery

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Nano Research 2022年第8期15卷 7190-7198页

作者： Jiaxu Li Junfeng Ren Caixia Li Pengxian Li Tingting Wu Shiwei Liu Lei Wang State Key Laboratory Base of Eco-chemical Engineering Taishan Scholar Advantage and Characteristic Discipline Team of Eco-chemical Process and TechnologyQingdao University of Science and TechnologyQingdao 266042China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042China

To conquer severe dendrites formation and side reactions of zinc metal anodes,which are serious obstacles for the practical applications of aqueous zinc ion battery(ZIB),herein,we develop a sodium allysulfonate(SAS)and acrylamide(AM)copolymer by radical polymerization process(crosslinking of C=C)as solid-state electrolyte.The interface kinetics is improved remarkably due to the high adhesion and excellent ion transferability of AM-SAS(AS)copolymers.Especially the sulfonic acid group in the hydrogel electrolyte can enhance the internal ionic conductivity effectively benefiting from its high affinity to Zn^(2+).Also,polymer chains realize re-regulation to Zn^(2+)flow in atomic-scale,thus leading to controllable deposition of Zn onto the dendrite-free Zn anodes.Consequently,the AS-1.5 electrolyte achieves ultra-stable Zn deposition/stripping behaviors with the lifespan over 1,000 h via the suppression of side-reactions and paralleled Zn deposition.High performances of Zn/Mn-doped V_(2)O_(5)(MnVO)(over 500 cycles)and Zn/diquinoxalino[2,3-a:2',3'-c]phenazine(HATN)(over 2,500 cycles)full cells demonstrate that the AS hydrogel electrolyte is a common approach for ZIBs under various conditions.This molecular regulation engineering opens a novel route for hydrogel electrolyte fabrication,where sulfonic groups perform as media of Zn^(2+)transfer.Therefore,high bulk ionic conductivity as well as excellent interface ion diffusion ability is obtained.

关键词： copolymer adhesion ionic conductivity dendrite-free interface kinetics

dendrite-free and stable Zn metal anodes with ZnO protective layer

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Science China(Technological Sciences) 2022年第10期65卷 2361-2368页

作者： HOU ZhenHua TAO HuaChao WANG JiaXu ZHANG LuLu YANG XueLin Hubei Provincial Collaborative Innovation Center for New Energy Microgrid College of Electrical Engineering&New EnergyChina Three Gorges UniversityYichang 443002China

Metallic Zn can be used as an anode for aqueous zinc-ion batteries due to its low redox potential,rich resources,and high theoretical capacity.However,its practical application is limited by dendrite growth and side reactions.Herein,a simple in-situ growth strategy was applied to fabricate a Zn anode with a ZnO protective layer(Zn/ZnO)to lengthen the cycle life and inhibit the dendrite growth and side reactions.At 1 mA h cm^(−2)capacity,Zn/ZnO exhibits long-time stability(2500 h)at 1 mA cm^(−2)and outstanding rate capability(1000 h at 10 mA cm^(−2))in symmetrical cells.Furthermore,the average coulombic efficiency of the Zn/ZnO//Ti cell is 99.4%,which is desirable at 5 mA cm^(−2).In addition,the Zn/ZnO//MnO_(2)cell can maintain a specific capacity of 167.2 mA h g^(−1)after 800 stable cycles.This work presents a simple fabrication method for Zn anode with excellent performance and suggests the huge possibilities of implementing practically rechargeable aqueous zinc-ion batteries.

关键词： aqueous zinc-ion batteries Zn anode ZnO protective layer dendrite-free