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Regulating the inner Helmholtz plane structure at the electrolyte-electrode interface for highly reversible aqueous Zn batteries

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Journal of Energy Chemistry 2024年第8期95卷 57-67页

作者： Jianghe Liu Sanlue Hu Hexin Guo Guobin Zhang Wen Liu Jianwei Zhao Shenhua Song Cuiping Han Baohua Li Shenzhen Key Laboratory on Power Battery Safety and Shenzhen Geim Graphene Center Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen Key Laboratory of Advanced Materials School of Materials Science and Engineering Harbin Institute of Technology Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen HUASUAN Technology Co. Ltd.

The development of aqueous Zn batteries is limited by parasitic water reactions,corrosion,and dendrite growth.To address these challenges,an inner Helmholtz plane（IHP） regulation method is proposed by employing low-cost,non-toxic maltitol as the electrolyte additive.The preferential adsorption behavior of maltitol can expel the water from the inner Helmholtz plane,and thus hinder the immediate contact between Zn metal and H2O.Meanwhile,strong interaction between maltitol and H2O molecules can restrain the activity of H2O.Besides,the "IHP adsorption effect" along with the low LUMO energy level of maltitol-CF3SO3-can promote the in-situ formation of an organic-inorganic complex solid electrolyte interface（SEI） layer.As a result,the hydrogen/oxygen evolution side reaction,corrosion,and dendrites issues are effectively suppressed,thereby leading to highly reversible and dendrite-free Zn plating/stripping.The Zn‖I2battery with hybrid electrolytes also demonstrates high electrochemical performance and ultralong cycling stability,showing a capacity retention of 75% over 20000 charge-discharge cycles at a large current density of 5 A g-1.In addition,the capacity of the device has almost no obvious decay over20000 cycles even at-30℃.This work offers a successful electrolyte regulation strategy via the IHP adsorption effect to design electrolytes for high-performance rechargeable Zn-ion batteries.

关键词： Adsorption effect dendrite suppression Inner Helmholtz plane SEI layer Zn||I2 battery

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Constructing a fluorinated interface layer enriched with Ge nanoparticles and Li-Ge alloy for stable lithium metal anodes

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Nano Research 2024年第6期17卷 5148-5158页

作者： Fulu Chu Jinwei Zhou Jiamin Liu Fengcheng Tang Liubin Song Feixiang Wu School of Metallurgy and Environment Engineering Research Center of the Ministry of Education for Advanced Battery MaterialsHunan Provincial Key Laboratory of Nonferrous Value-added MetallurgyCentral South UniversityChangsha 410083China Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation School of Chemistry and Chemical EngineeringChangsha University of Science and TechnologyChangsha 410004China School of Materials Science&Engineering University of JinanJinan 250022China

Lithium metal batteries(LMBs)based on metallic Li exhibit high energy density to be competent for advanced energy storage applications.However,the unstable solid electrolyte interphase(SEI)layer due to continuous decomposition of electrolytes,and the attendant problem of Li dendrite growth frustrate their commercialization process.Herein,a hybrid SEI comprising abundant LiF,lithiophilic Li-Ge alloy,and Ge nanoparticles is constructed via a simple brush coating method.This fluorinated interface layer with embedded Ge-containing components isolates the Li anode from the corrosive electrolyte and facilitates homogenous Li nucleation as well as uniform growth.Consequently,the modified Li anode exhibits remarkable stability without notorious Li dendrites,delivering stable cycling lives of more than 1000 h for symmetric Li||Li cells and over 600 cycles for Li||Cu cells at 1 mA·cm^(−2).Moreover,the reinforced Li anodes endow multiple full-cell architectures with dramatically improved cyclability under different test conditions.This work provides rational guidance to design an artificial hybrid SEI layer and would stimulate more ideas to solve the dendrite issue and promote the further development of advanced LMBs.

关键词： lithium metal anode artificial solid electrolyte interphase(SEI) dendrite suppression lithium fluoride Li-Ge alloy

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Recent developments in three-dimensional Zn metal anodes for battery applications

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InfoMat 2024年第1期6卷 1-30页

作者： Jianyu Chen Yizhou Wang Zhengnan Tian Jin Zhao Yanwen Ma Husam N.Alshareef State Key Laboratory of Organic Electronics and Information Displays(KLOEID)and Jiangsu Key Laboratory for Biosensors Institute of Advanced Materials(IAM)Nanjing University of Posts&Telecommunications(NUPT)Nanjingthe People's Republic of China Materials Science and Engineering King Abdullah University of Science and Technology(KAUST)ThuwalSaudi Arabia Suzhou Vocational Institute of Industrial Technology Suzhouthe People's Republic of China

Aqueous zinc(Zn)ion batteries(AZIBs)are regarded as one of the promising candidates for next-generation electrochemical energy storage systems due to their low cost,high safety,and environmental friendliness.However,the commercialization of AZIBs has been severely restricted by the growth of dendrite at the Zn metal anode.Tailoring the planar-structured Zn anodes into threedimensional(3D)structures has proven to be an effective way to modulate the plating/stripping behavior of Zn anodes,resulting in the suppression of dendrite formation.This review provides an up-to-date review of 3D structured Zn metal anodes,including working principles,design,current status,and future prospects.We aim to give the readers a comprehensive understanding of 3D-structured Zn anodes and their effective usage to enhance AZIB performance.

关键词： 3D metal anodes aqueous Zn ion batteries dendrite suppression Zn dendrite Zn metal anodes

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Fast Zn^(2+)mobility enabled by sucrose modified Zn^(2+)solvation structure for dendrite-free aqueous zinc battery

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Nano Research 2023年第3期16卷 3839-3846页

作者： Yufang Cao Xiaohui Tang Linge Li Haifeng Tu Yuzhen Hu Yingying Yu Shuang Cheng Hongzhen Lin Liwen Zhang Jiangtao Di Yongyi Zhang Meinan Liu School of Nano-Tech and Nano-Bionics University of Science and Technology of ChinaHefei 230026China Key Laboratory of Multifunctional Nanomaterials and Smart Systems Advanced Materials DivisionSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Division of Nanomaterials and Jiangxi Key Lab of Carbonene Materials Jiangxi Institute of NanotechnologyNanchang 330200China

Aqueous zinc battery has been regarded as one of the most promising energy storage systems due to its low cost and environmental benignity.However,the safety concern on Zn anodes caused by uncontrolled Zn dendrite growth in aqueous electrolyte hinders their application.Herein,sucrose with multi-hydroxyl groups has been introduced into aqueous electrolyte to modify Zn^(2+)solvation environment and create a protection layer on Zn anode,thus effectively retarding the growth of zinc dendrites.Atomistic simulations and experiments confirm that sucrose molecules can enter into the solvation sheath of Zn^(2+),and the as-formed unique solvation structure enhances the mobility of Zn^(2+).Such fast Zn^(2+)kinetics in sucrose-modified electrolyte can successfully suppress the dendrite growth.With this sucrose-modified aqueous electrolyte,Zn/Zn symmetric cells present more stable cycle performance than those using pure aqueous electrolyte;Zn/C cells also deliver an impressive higher energy density of 129.7 Wh·kg^(−1)and improved stability,suggesting a great potential application of sucrose-modified electrolytes for future Zn batteries.

关键词： solvation structure Zn^(2+)mobility dendrite suppression sucrose

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Polyanionic hydrogel electrolyte enables reversible and durable Zn anode for efficient Zn-based energy storage

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Journal of Energy Chemistry 2023年第11期86卷 373-381,I0008页

作者： Chunjiang Jin Congcong Yang Hongyu Mi Chenchen Ji Fengjiao Guo Chengzhe Liu Ziqiang Liu Nianjun Yang State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources School of Chemical Engineering and TechnologyXinjiang UniversityUrumqi 830017XinjiangChina Department of Chemistry Hasselt UniversityDiepenbeek 3590Belgium

Aqueous Zn-ion energy storage systems,which are expected to be integrated into intelligent electronics as a secure power supply,suffer poor reversibility of Zn anodes,predominantly associated with dendritic growth and side reactions.This study introduces a polyanionic strategy to address these formidable issues by developing a hydrogel electrolyte(PACXHE)with carboxyl groups.Notably,the carboxyl groups within the hydrogel structure establish favorable channels to promote the transport of Zn^(2+)ions.They also expedite the desolvation of hydrated Zn^(2+)ions,leading to enhanced deposition kinetics.Additionally,these functional groups confine interfacial planar diffusion and promote preferential deposition along the(002)plane of Zn,enabling a smooth surface texture of the Zn anode.This multifaceted regulation successfully achieves the suppression of Zn dendrites and side reactions,thereby enhancing the electrochemical reversibility and service life during plating/stripping cycles.Therefore,such an electrolyte demonstrates a high average Coulombic efficiency of 97.7%for 500 cycles in the Zn‖Cu cell and exceptional cyclability with a duration of 480 h at 1 mA cm^(-2)/1 mA h cm^(-2)in the Zn‖Zn cell.Beyond that,the Zn-ion hybrid micro-capacitor employing PACXHE exhibits satisfactory cycling stability,energy density,and practicality for energy storage in flexible,intelligent electronics.The present polyanionic-based hydrogel strategy and the development of PACXHE represent significant advancements in the design of hydrogel electrolytes,paving the way for a more sustainable and efficient future in the energy storage field.

关键词： Polyanionic hydrogel electrolyte Zinc anode issues dendrite suppression Electrochemical performance Zinc-ionhybrid micro-capacitor

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Double interface regulation: Toward highly stable lithium metal anode with high utilization

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InfoMat 2022年第7期4卷 147-159页

作者： Guanyao Wang Ming Zhu Ying Zhang Chan Song Xiaolong Zhu Zhongyi Huang Yuanjun Zhang Fangfang Yu Gang Xu Minghong Wu Hua-Kun Liu Shi-Xue Dou Chao Wu School of Environmental and Chemical Engineering Shanghai UniversityShanghaiChina Institute for Superconducting&Electronic Materials Australian Institute of Innovative MaterialsUniversity of WollongongWollongongNew South WalesAustralia School of Chemistry and Molecular Engineering Nanjing Tech UniversityNanjingJiangsuChina Key Laboratory of Organic Compound Pollution Control Engineering(MOE) Shanghai UniversityShanghaiChina

The undesirable Li dendrite growth and other knock-on issues have signifi-cantly plagued the application of Li metal anodes(LMAs).Herein,we report that the synergistic regulation of double interfaces adjacent to the metallic Li anode can effectively prevent the dendritic Li growth,significantly improving the cycling performance of LMAs under harsh conditions including high cur-rent density and high depth of discharge.Thorough comparison of electrolytes demonstrated that 1 M lithium bis(fluorosulfonyl)imide(LiFSI)in 1,2-dimethoxyethane(DME)can yield a robust and lithiophobic LiF-rich upper interface(solid electrolyte interphase).Besides,the Sb-based buffer layer forms a lithiophilic lower interface on current collector.The synergy of the upper and lower interfacial engineering plays an important role for outstanding cyclability of LMAs.Consequently,the plating/stripping of Li can be stably repeated for 835 and 329 cycles with an average Coulombic efficiency(CE)above 99%at 1 and 3 mA h cm?2,respectively.Surprisingly,the Li||Li symmetric cell can even withstand the baptism of current density up to 20 mA cm?2.The excellent performance validates that the facile synergistic regulating of interfaces adjacent to the metallic Li anode provides an effective pathway to stabilize LMAs.

关键词： dendrite suppression electrolytes lithium metal anodes nucleation buffer layer solid electrolyte interphase

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Hybrid solid electrolyte enabled dendrite-free Li anodes for high-performance quasi-solid-state lithium-oxygen batteries

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National Science Review 2021年第2期8卷 123-133页

作者： Jin Wang Gang Huang Jun-Min Yan Jin-Ling Ma Tong Liu Miao-Miao Shi Yue Yu Miao-Miao Zhang Ji-Lin Tang Xin-Bo Zhang Key Laboratory of Automobile Materials Ministry of EducationDepartment of Materials Science and EngineeringJilin University State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences Materials Science and Engineering Physical Science and Engineering DivisionKing Abdullah University of Science and Technology State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences

The dendrite growth of Li anodes severely degrades the performance of lithium-oxygen(Li-O2) batteries.Recently, hybrid solid electrolyte(HSE) has been regarded as one of the most promising routes to tackle this problem. However, before this is realized, the HSE needs to simultaneously satisfy contradictory requirements of high modulus and even, flexible contact with Li anode, while ensuring uniform Li+distribution. To tackle this complex dilemma, here, an HSE with rigid Li1.5Al0.5Ge1.5(PO4)3(LAGP)core@ultrathin flexible poly(vinylidene fluoride-hexafluoropropylene)(PVDF-HFP) shell interface has been developed. The introduced large amount of nanometer-sized LAGP cores can not only act as structural enhancer to achieve high Young’s modulus but can also construct Li+diffusion network to homogenize Li+distribution. The ultrathin flexible PVDF-HFP shell provides soft and stable contact between the rigid core and Li metal without affecting the Li+distribution, meanwhile suppressing the reduction of LAGP induced by direct contact with Li metal. Thanks to these advantages, this ingenious HSE with ultra-high Young’s modulus of 25 GPa endows dendrite-free Li deposition even at a deposition capacity of 23.6 m Ah.Moreover, with the successful inhibition of Li dendrites, the HSE-based quasi-solid-state Li-O2battery delivers a long cycling stability of 146 cycles, which is more than three times that of gel polymer electrolyte-based Li-O2battery. This new insight may serve as a starting point for further designing of HSE in Li-O2batteries, and can also be extended to various battery systems such as sodium-oxygen batteries.

关键词： lithium-oxygen batteries dendrite suppression Li anodes hybrid solid electrolyte LAGP PVDF-HFP

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dendrite‑Free and Stable Lithium Metal Battery Achieved by a Model of Stepwise Lithium Deposition and Stripping

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Nano-Micro Letters 2021年第11期13卷 155-167页

作者： Tiancun Liu Jinlong Wang Yi Xu Yifan Zhang Yong Wang Department of Chemical Engineering School of Environmental and Chemical EngineeringShanghai University99 Shangda RoadShanghai 200444People’s Republic of China Key Laboratory of Organic Compound Pollution Control Engineering(MOE) 99 Shangda RoadShanghai 200444People’s Republic of China

The uncontrolled formation of lithium(Li)dendrites and the unnecessary consumption of electrolyte during the Li plating/stripping process have been major obstacles in developing safe and stable Li metal batteries.Herein,we report a cucumber-like lithiophilic composite skeleton(CLCS)fabricated through a facile oxidationimmersion-reduction method.The stepwise Li deposition and stripping,determined using in situ Raman spectra during the galvanostatic Li charging/discharging process,promote the formation of a dendrite-free Li metal anode.Furthermore,numerous pyridinic N,pyrrolic N,and CuxN sites with excellent lithiophilicity work synergistically to distribute Li ions and suppress the formation of Li dendrites.Owing to these advantages,cells based on CLCS exhibit a high Coulombic efficiency of 97.3%for 700 cycles and an improved lifespan of 2000 h for symmetric cells.The full cells assembled with LiFePO_(4)(LFP),SeS_(2) cathodes and CLCS@Li anodes demonstrate high capacities of 110.1 mAh g^(−1) after 600 cycles at 0.2 A g^(−1) in CLCS@Li|LFP and 491.8 mAh g^(−1) after 500 cycles at 1 A g^(−1) in CLCS@Li|SeS2.The unique design of CLCS may accelerate the application of Li metal anodes in commercial Li metal batteries.

关键词： Lithiophilic skeleton Stepwise Li deposition and stripping dendrite suppression Lithium metal battery Electrochemical properties

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Heterogeneous electrolyte membranes enabling double-side stable interfaces for solid lithium batteries

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Journal of Energy Chemistry 2021年第9期30卷 162-168页

作者： Shuang Mu Weilin Huang Wuhui Sun Ning Zhao Mengyang Jia Zhijie Bi Xiangxin Guo College of Physics Qingdao UniversityQingdao 266071ShandongChina

The solid polymer electrolyte(SPE) is one of the most promising candidates for building solid lithium batteries with high energy density and safety due to its advantages of flexibility and light-weight.However,the conventional monolayered electrolytes usually exhibit unstable contacts with either high-voltage cathodes or Li-metal anodes during cell operation.Herein,heterogeneous dual-layered electrolyte membranes(HDEMs) consisting of the specific functional polymer matrixes united with the designed solid ceramic fillers are constructed to address the crucial issues of interfacial instability.The electrolyte layers composed of the high-conductivity and oxidation-resistance polyacrylonitrile(PAN) combined with Li_(0.33)La_(0.557)TiO_(3) nanofibers are in contact with the high-voltage cathodes,achieving the compatible interface between the cathodes and the electrolytes.Meanwhile,the electrolyte layers composed of the highstability and dendrite-resistance polyethylene oxide(PEO) with Li_(6.4)La_(3) Zr_(1.4)Ta_(0.6)O_(12) nanoparticles are in contact with the Li-metal anodes,aiming to suppress the dendrite growth,as well as avoid the passivation between the PAN and the Li-metal.Consequently,the solid LiNi_(0.6)Co_(0.2)Mn_(0.2)O2‖Li full cells based on the designed HDEMs show the good rate and cycling performance,i.***.the discharge capacity of 170.1 mAh g^(-1) with a capacity retention of 78.2% after 100 cycles at 0.1 C and 30℃.The results provide an effective strategy to construct the heterogeneous electrolyte membranes with double-side stable electrode/-electrolyte interfaces for the high-voltage and dendrite-free solid lithium batteries.

关键词： Solid electrolytes High-voltage cathodes dendrite suppression Solid lithium batteries

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