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Novel 2D bifunctional layered rare-earth hydroxides@GO catalyst as a functional interlayer for improved liquid-solid conversion of polysulfides in lithium-sulfur batteries

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Chinese Chemical Letters 2024年第5期35卷 434-440页

作者： Haodong Wang Xiaoxu Lai Chi Chen Pei Shi Houzhao Wan Hao Wang Xingguang Chen Dan Sun CAS Key Laboratory of Design and Assembly of functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Fujian Normal UniversityFuzhou 350007China Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China School of Microelectronics Hubei UniversityWuhan 430062China Xiamen Key Laboratory of Rare Earth Photoelectric functional Materials Xiamen 361021China

The detrimental“shuttle effect”of lithium polysulfides(LiPSs)together with sluggish multi-order reaction kinetics are the main drawbacks hindering lithium-sulfur(Li-S)batteries from commercial success.Here,we first propose the implementability of layered rare-earth hydroxides(LREHs)in Li-S batteries to optimize electrochemical performance.In this work,a two-dimensional(2D)rare-earth-based composite constructed by the layered gadolinium hydroxy chloride[Gd_(2)(OH)_(5)(H_(2)O)_(n)]Cl nanoplates(LGdH NPs)and graphene oxide(GO)was designed as a sulfur immobilizer for Li-S batteries.Combining the experimental results and density functional theory(DFT)calculations,it is revealed that the LGdH@GO composite not only provides a strong anchoring of the intermediates during cycling,but also acts as an effective catalyst to accelerate the liquid-solid conversion of polysulfides.The Li-S batteries assembled by LGdH@GO modified separators delivered a superior rate performance with a specific capacity of 605.34 mAh/g at 5 C,as well as excellent cycle stability with a decay rate of 0.087%over 500 cycles at 2 C.This study provided a deep understanding of the mechanism to suppress the“shuttle effect”by the LREHs,and a guide to design effective functional interlayers for high-performance Li-S batteries with excellent electrocatalytic activity.

关键词： Lithium-sulfur batteries functional separator Layered rare-earth hydroxides Shuttle effect Adsorption Catalysis

2D spinel ZnCo_(2)O_(4) microsheet-coated functional separator for promoted redox kinetics and inhibited polysulfide dissolution

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Journal of Energy Chemistry 2021年第4期30卷 468-475页

作者： Jeong Seok Yeon Tae Ho Park Young Hun Ko Periyasamy Sivakumar Jun Su Kim Youngkywon Kim Ho Seok Park School of Chemical Engineering Sungkyunkwan UniversitySuwon 16419Gyeonggi-doRepublic of Korea Advanced Batteries Research Center Korea Electronics Technology InstituteSeongnam 13509Gyeonggi-doRepublic of Korea Department of Health Sciences and Technology Samsung Advanced Institute for Health Sciences and Technology(SAIHST)Sungkyunkwan UniversitySuwon 16419Gyeonggi-doRepublic of Korea Department of Chemistry Dongguk University-Seoul CampusJung-gu 04620 SeoulRepublic of Korea

Lithium-sulfur(Li-S)batteries are receiving increasing attention as one of the potential next-generation batteries,owing to their high energy densities and low cost.However,practical Li-S batteries with high energy densities are extremely hindered by the sulfur loss,low Coulombic efficiency,and short cycling life originating from the polysulfide(LiPS)shuttle.In this study,two-dimensional(2D)ZnCo_(2)O_(4) microsheets fabricated by a facile hydrothermal process are employed to modify the separator,for improving the electrochemical performances of Li-S cells.The resulting 2D Zn Co_(2)O_(4)-coated separator features a coating thickness of approximately 10 lm,high ionic conductivity of 1.8 m S/cm,and low mass loading of 0.2 mg/cm^(2).This 2D ZnCo_(2)O_(4)-coated separator effectively inhibits Li PS shuttle by a strong chemical interaction with Li PS as well as promotes the redox kinetics by Zn CO2O4-coated layers,as determined by X-ray photoelectron spectroscopy analysis,self-discharge,time-dependent permeation test,Li symmetric cell test,and Li2S nucleation analyses.Consequently,the Li-S batteries based on the 2D Zn Co_(2)O_(4)-coated separator exhibit a high initial discharge capacity of 1292.2 m Ah/g at 0.1 C.Moreover,they exhibit excellent long cycle stability at 1 and 2 C with capacity retention of 84%and 86%even after800 cycles,corresponding to a capacity fading rate of 0.020%and 0.016%per cycle,respectively.Effectively,these Li-S cells with a high sulfur loading at 5.3 mg/cm^(2) and low electrolyte concentration of 9 l L/mg deliver a high discharge capacity of 4.99 m Ah/cm^(2) after 200 cycles at 0.1 C.

关键词： Lithium sulfur batteries functional separator 2D microsheet Polysulfide Redox kinetics

Regulating surface chemistry of separator with LiF for advanced Li-S batteries

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Frontiers in Energy 2022年第4期16卷 601-606页

作者： Shuai WANG Fanyang HUANG Shuhong JIAO Yulin JIE Yawei CHEN Shiyang WANG Ruiguo CAO Hefei National Laboratory for Physical Science at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Lithium-sulfur(Li-S)batteries have attracted intensive attention owing to their ultrahigh theoretical energy density.Nevertheless,the practical application of Li-S batteries is prevented by uncontrollable shuttle effect and retarded reaction kinetics.To address the above issues,lithium fluoride(LiF)was employed to regulate the surface chemistry of routine separator.The functional separator demonstrates a great ability to suppress active S loss and protect lithium anode.This work provides a facile strategy for the development of advanced Li-S batteries.

关键词： Li-S batteries LiF functional separator

Three-in-one LaNiO_(3) functionalized separator boosting electrochemical stability and redox kinetics for high-performance Li-S battery

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Journal of Energy Chemistry 2023年第7期82卷 581-591,I0013页

作者： Weiyu Wang Mingxiu Hou Fangqian Han Di Yu Jie Liu Qian Zhang Fengli Yu Lei Wang Maoshuai He State Key Laboratory Base of Eco-chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Weifang Key Laboratory of Green Processing of separator for Chemical Power Sources School of Chemistry and EngineeringWeifang Vocational CollegeWeifang 261108ShandongChina Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

The lithium-sulfur(Li-S)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy density.However,the poor redox kinetics and the"shuttle effect"of polysulfides severely restrict the use of Li-S batteries in practical applications.Herein,a novel bimetallic LaNiO_(3) functional material with high electrical conductivity and catalytic property is prepared to act as a high-efficiency polysulfide shuttling stopper.The three LaNiO_(3) samples with different physical/chemical characteristics are obtained by controlling the calcination temperature.In conjunction with the high electrical conductivity and excellent catalytic properties of the as-prepared materials,the appropriate chemisorption toward polysulfides offers great potential to enhance electrochemical stability for highperformance Li-S batteries.Particularly,the Li-S cell with the separator modified by such functional material gives a specific capacity of 658 mA h g^(-1) after 500 cycles at a high current density of 2 C.Even with high sulfur loading of 6.05 mg cm^(-2),the Li-S battery still exhibits an areal specific capacity of 2.81 m A h cm^(-2)after 150 cycles.This work paves a new avenue for the rational design of materials for separator modification in high-performance Li-S batteries.

关键词： Li-S battery functional separator Catalytic property Electrochemical stability Redox kinetics

Regulating the growth of lithium dendrite by coating an ultra-thin layer of gold on separator for improving the fast-charging ability of graphite anode

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Journal of Energy Chemistry 2022年第4期31卷 467-473页

作者： Shuaishuai Yan Xiaoxia Chen Pan Zhou Peican Wang Hangyu Zhou Weili Zhang Yingchun Xia Kai Liu The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

With the ever-growing application of lithium-ion batteries(LIBs), their fast-charging technology has attracted great interests of scientists. However, growth of lithium dendrites during fast charge of the bat teries with high energy density may pose great threats to the operation and cause serious safety issues Herein, we prepared a functional separator with an ultra-thin(20 nm) layer of Au nanoparticles deposited by evaporation coating method which could regulate growth direction and morphology of the lithium dendrites, owing to nearly zero overpotential of lithium meal nucleation on lithiated Au. Once the Li den drites are about to form on the graphite anode during fast charging(or lithiation), they plate predomi nantly on the Au deposited separator rather than on the graphite. Such selective deposition does no compromise the electrochemical performance of batteries under normal cycling. More importantly, i enables the better cycling stability of batteries at fast charge condition. The Li/Graphite cells with Au nanoparticles coated separator could cycle stably with a high areal capacity retention of 90.5% over 95 cycles at the current density of 0.72 m A cm^(-2). The functional separator provides an effective strategy to adjust lithium plating position at fast charge to ensure high safety of batteries without a compromise on the energy density of LIBs.

关键词： Fast-charging functional separator Lithium-ion batteries Dendrites Safety

Li3N film modified separator with homogenization effect of lithium ions for stable lithium metal battery

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Progress in Natural Science:Materials International 2021年第6期31卷 845-851页

作者： Zhongyun Yan Cheng Zhou Cheng Li Yan Li Chunli Shen Kaijian Yan Xu Xu International School of Materials Science and Engineering State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

Lithium metal anode with high theoretical capacity is considered to be one of the most potential anode materials of the next generation. However, the growth of lithium dendrite seriously affects the application of lithium metal anode and the development of lithium metal batteries(LMBs). Herein, an ultrathin LiN film modified separator to homogenize the lithium ions and protect the lithium metal anode was reported. Due to the intrinsic properties of LiN, the functional separator possessed good thermal stability, mechanical properties and electrolyte wettability, and the homogenization of the lithium ion was realized without increasing the interface impedance. With this functional separator, the Li/Li symmetrical cell could achieve a long cycle with low overpotential for 1000 h at a current density of 1 m A cm. Furthermore, when the full battery was assembled with Li FePOand the discharge capacity could be maintained at 151 m Ah gafter 400 cycles at 1 C. In addition, the full battery also showed good rate performance, and provided a high discharge capacity of 114 m Ah gat 5 C.

关键词： functional separator Solid electrolyte interface Physical vapor deposition Li metal anode