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Elucidating the suppression of lithium dendrite growth with a void-reduced anti-perovskite solid-state electrolyte pellet for stable lithium metal anodes

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Journal of Energy Chemistry 2023年第2期77卷 62-69,I0003页

作者： Yu YeXinyan Ye Haoxian Zhu juncao bian Haibin Lin Jinlong Zhu Yusheng Zhao Shenzhen Key Laboratory of Solid State Batteries Southern University of Science and TechnologyShenzhen 518055GuangdongChina Academy for Advanced Interdisciplinary Studies&Department of Physics Southern University of Science and TechnologyShenzhen 518055GuangdongChina Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and TechnologyShenzhen 518055GuangdongChina Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices Southern University of Science and TechnologyShenzhen 518055GuangdongChina

Solid-state lithium-metal batteries,with their high theoretical energy density and safety,are highly promising as a next-generation battery *** the alternatives proposed as solid-state electrolyte,lithium-rich anti-perovskite(Li RAP)materials have drawn the most interest because of high theoretical Li^(+)conductivity,low cost and easy *** solid-state electrolytes are believed to have the potential to physically inhibit the lithium dendrite growth,lithium-metal batteries still suffer from the lithium dendrite growth and thereafter the short *** voids in practical Li RAP pellets are considered as the root ***,we show that reducing the voids can effectively suppress the lithium dendrite *** voids in the pellet resulted in an irregular Li^(+)flux distribution and a poor interfacial contact with lithium metal anode;and hence the ununiform lithium ***,the lithium-metal symmetric cell with void-reduced Li_(2)OHCl-HT pellet was able to display excellent cycling performance(750 h at 0.4 m A cm^(-2))and stability at high current density(0.8 m A cm^(-2)for 120 h).This study provides not only experimental evidence for the impact of the voids in Li RAP pellets on the lithium dendrite growth,but also a rational pellet fabrication approach to suppress the lithium dendrite growth.

关键词： Llithium-rich anti-perovskite Solid-state electrolytes Void-reduced pellets Lithium dendrites Lithium metal anodes

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Electrolyte solvation chemistry for lithium-sulfur batteries with electrolyte-lean conditions

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Journal of Energy Chemistry 2021年第4期30卷 80-91页

作者： Long Kong Lihong Yin Fei Xu juncao bian Huimin Yuan Zhouguang Lu Yusheng Zhao Academy for Advanced Interdisciplinary Studies Southern University of Science and TechnologyShenzhen 518055GuangdongChina Department of Physics Southern University of Science and TechnologyShenzhen 518055GuangdongChina Department of Materials Science and Engineering Guangdong Provincial Key Laboratory of Energy Materials for Electric PowerSouthern University of Science and TechnologyShenzhen 518055GuangdongChina Technische Universität Dresden Bergstrasse 6601062DresdenGermany

Lithium-sulfur(Li-S)batteries possess overwhelming energy density of 2654 Wh kg-1,and are considered as the next-generation battery technology for energy demanding *** electrolytes are ubiquitously employed in cells to ensure sufficient redox kinetics and preclude the interference of the electrolyte depletion due to side reactions with the lithium metal *** strategy is capable of enabling long-lasting,high-capacity and excellent-rate battery performances,but it mask the requirements of practical Li-S batteries,where high-sulfur-loading/content and lean electrolyte are prerequisite to realize the energy-dense Li-S *** and highly solvating electrolytes have emerged as effective yet simple approaches to decrease the electrolyte/sulfur ratio through altering sulfur species and exerting new reaction *** solvating electrolytes are characterized by few free solvents to solvate lithium polysulfides,rendering a quasi-solid sulfur conversion and decoupling the reaction mechanisms from electrolyte quantity used in cells;while highly solvating electrolytes adopt highdonicity or high-permittivity solvents and take their advantages of strong solvation ability toward polysulfide intermediates,thereby favoring the polysulfide formation and stabilizing unique radicals,which subsequently accelerate redox *** solvation chemistry approaches have their respective features to allow the operation of cells under electrolyte-starved *** Review discusses their unique features and basic physicochemical properties in the working Li-S batteries,presents remaining technical and scientific issues and provides future directions for the electrolyte chemistry to attain highenergy Li-S batteries.

关键词： Li-S batteries Solvation chemistry Energy density Polysulfides Lean electrolyte

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Lithium polysulfide solvation and speciation in the aprotic lithium-sulfur batteries

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Particuology 2024年第6期89卷 238-245页

作者： Jinhao Zhang Qingshan Fu Peng Li Ruibo Linghu Xiaozhong Fan Haibin Lin juncao bian Songbai Han Gengzhi Sun Long Kong Frontiers Science Center for Flexible Electronics and Xi’an Institute of Flexible Electronics Northwestern Polytechnical UniversityXi’an710129China China Automotive Innovation Corporation Nanjing211100China Academy for Advanced Interdisciplinary Studies Southern University of Science and TechnologyShenzhen518055China Institute of Advanced Materials Nanjing Tech UniversityNanjing211816China

Fingerprinting sulfur speciation in aprotic electrolytes is a key to understand fundamental chemistry and design well-performing lithium–sulfur(Li–S)*** polysulfide(LiPS)dissolution and deposition in ether-based electrolytes during redox reactions have been probed and established by spectroscopy and ***,detailed LiPS structure and solvation properties influenced by conventional and newly developed electrolytes remain elusive,which exert fundamental challenges and practical difficulties in decoupling battery performance from electrolyte *** perspective aims to provide timely information to uncover underlying mechanisms that rein in sulfur speciation by considering the charge density of LiPSs and the coordination strength of solvents/*** discussion starts with unlocking the baseline electrolyte formulation to investigate its role in LiPS formation and *** that,the term coordination strength is used instead of donor number and dielectric constant to describe interactions between solvents and LiPSs and to reveal LiPS structure *** work is expected to encourage the discovery of new electrolyte working mechanisms to develop energy-dense and power-intensive Li–S batteries.

关键词： Sulfur speciation Redox kinetics Coordination strength Solvation chemistry Lithium-sulfur batteries

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A fiber-reinforced solid polymer electrolyte by in situ polymerization for stable lithium metal batteries

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Nano Research 2023年第7期16卷 9259-9266页

作者： Yifan Xu Ruo Zhao Lei Gao Tingsong Gao Wenjuan Wang juncao bian Songbai Han Jinlong Zhu Qiang Xu Yusheng Zhao Institute for Advanced Study Shenzhen UniversityShenzhen 518055China Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and DevicesAcademy for Advanced Interdisciplinary StudiesSouthern University of Science and TechnologyShenzhen 518055China Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials Department of Materials Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China School of Materials Science and Engineering Peking UniversityBeijing 100871China

Solid polymer electrolytes(SPEs)by in situ polymerization are attractive due to their good interfacial contact with *** reported in situ polymerized SPEs,however,suffer from the low polymerization degree that causes poor mechanical strength,Li dendrite penetration,and performance decay in Li-metal *** highly polymerized SPEs are more stable than lowly polymerized ones,they are restricted by their sluggish long-chain mobility and poor ionic *** this work,a three-dimensional fibrous membrane with ion selectivity was prepared and used as a functional filler for the in situ formed *** obtained SPE has high stability due to its high polymerization degree after the long-term heating *** fibrous membrane plays a vital role in improving the SPE’s *** rich anion-adsorption sites on the fibrous membrane can alleviate the polarization effect and benefit a uniform current distribution at the *** fibrous nanostructure can efficiently interact with the polymeric matrix,providing rich hopping sites for fast Li+***,the obtained SPE enables a uniform Li deposition and long-term cycling performance in Li-metal *** work reported an in situ formed SPE with both high polymerization degree and ionic conductivity,paving the way for designing high-performance SPEs with good comprehensive properties.

关键词： solid polymer electrolytes fibrous solid filler metal-organic frameworks in situ polymerization ion selectivity

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Effects of fluorination on crystal structure and electrochemical performance of antiperovskite solid electrolytes

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Journal of Energy Chemistry 2023年第2期77卷 521-528,I0013页

作者： Lei Gao Manrong Song Ruo Zhao Songbai Han Jinlong Zhu Wei Xia juncao bian Liping Wang Song Gao Yonggang Wang Ruqiang Zou Yusheng Zhao School of Materials Science and Engineering Peking UniversityBeijing 100871China Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and DevicesAcademy for Advanced Interdisciplinary StudiesSouthern University of Science and TechnologyShenzhen 518055GuangdongChina Institute for Advanced Study Shenzhen UniversityShenzhen 518055GuangdongChina

The development of all-solid-state lithium batteries(ASSLBs)depends on exploiting solid-state electrolytes(SSEs)with high ionic conductivity and electrochemical *** is generally considered to be an effective strategy to improve the ionic conductivity and electrochemical stability of inorganic ***,we report the partial fluorination of the chlo rine sites in an antiperovskite,by which the orthorhombic Li_(2)OHCl was transformed into cubic Li_(2)OHCl_(0.9)F_(0.1),resulting in a fourfold increase in ionic conductivity at 30℃.The ab initio molecular dynamics simulations suggest that both the crystal symmetry and the anions electronegativity influence the diffusion of Li+in the antiperovskite ***,from the perspective of experiments and calculations,it is confirmed that fluorination is a feasible method to improve the electrochemical stability of antiperovskite *** LiFePO_(4)|Li cell based on Li_(2)OHCl_(0.9)F_(0.1) is also assembled and exhibits stable cycle performance,which indicates that fluorination of antiperovskite SSEs is an effective way to produce high-performance SSEs for practical application of ASSLBs.

关键词： Antiperovskite Solid-state electrolyte Fluorination Ionic conductivity

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