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Difunctional NH_(2)-modified MOF supporting plentiful ion channels and stable lif-rich sei construction via organocatalysis for all-solid-state lithium metal batteries

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Journal of Materials Science & Technology 2023年第5期136卷 140-148页

作者： Xuanyi Zhou Chenghan Li Biao Zhang Fenfen Huang Pan Zhou Xinming Wang Zengsheng Ma Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education and School of Materials Science and EngineeringXiangtan UniversityXiangtan 411105China

As an essential part of the performance improvement of lithium metal batteries,the acquisition of dense(lif-rich solid electrolyte interphase(sei))has always been an urgent problem to be ***,we synthesized Zeolitic Imidazolate Frameworks(ZIFs)modified by two different functional groups(-NH_(2),-CH_(3))and used them as the fillers of polyethylene oxide(PEO)composite solid electrolytes to explore the catalytic effect of groups on lif generation at the Li/electrolytes *** a lifePO 4||SPE||Li cell test,the PEO-ZIF-NH_(2)with lif-rich sei exhibits enhanced cycling performance,which was 3.8 times longer than that of PEO-ZIF-CH_(3).The formation mechanism of lif-rich sei was investigated using first-principles calculation,revealing that ZIFs-NH_(2)makes the C-F bond in TFSI-longer compared with ZIFs-CH_(3),which leads to easier breakage of the C-F bond and promoted the formation of *** simple design idea of using organic catalysis to generate more stable sei provides a new aspect for preparing high-performance lithium metal batteries.

关键词： lif-rich sei Organic catalysis Functional groups Hydrogen bond Difunctional MOF

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Tailoring fluorine-rich solid electrolyte interphase to boost high efficiency and long cycling stability of lithium metal batteries

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Science China Chemistry 2023年第7期66卷 2121-2129页

作者： Tianyang Xue Ji Qian Xingming Guo Yi Chen Kaixin Yu Tianyang Yu Yao Li Li Li Feng Wu Renjie Chen Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Institute of Advanced Technology Beijing Institute of TechnologyJinan 250300China Collaborative Innovation Center of Electric Vehicles in Beijing Beijing 100081China

Lithium metal batteries(LMBs)are regarded as the most promising next-generation battery system due to their high energy ***,Li dendrite growth and low Coulombic efficiency(CE)of Li metal anodes limit their *** solid electrolyte interphase(sei)is an extremely effective method to solve these problems and using electrolyte additives to regulate the sei is one of the most effective ***,we study the feasibility of trans-difluoroethylene carbonate(DFEC)used as the solvent additive in conventional ether electrolyte,which has excellent anti-reduction stability against Li *** result shows that a Li/Cu half-cell with the modified electrolyte can be steadily cycled for 300 cycles with an average CE of 97.41%at the current density of 0.5 m A cm^(-2)and with 97.1%for 140 cycles at 1 m A cm^(-2).Besides,the Li/LFP full cell with the modified electrolyte displays an improved capacity retention of 94.55%after 520 cycles with an average CE of 99.74%at 1 *** contrast,the capacity retention of 56.2%and CE of 99.15%is obtained for the cell with pure ether *** SEM images show that the DFEC enables dense Li deposition,and the FTIR and XPS spectra confirm the formation of Li Frich sei with the *** work demonstrates the feasibility of using DFEC as the solvent additive in ether electrolyte to construct Li F-rich sei,and it will provide important insight in developing high-performance electrolytes for LMBs.

关键词： lithium metal batteries ether electrolyte trans-difluoroethylene carbonate lif-rich sei dense Li deposition

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Diluent decomposition-assisted formation of Li F-rich solid-electrolyte interfaces enables high-energy Li-metal batteries

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Journal of Energy Chemistry 2023年第3期78卷 71-79,I0003页

作者： Junbo Zhang Haikuo Zhang Ruhong Li Ling Lv Di Lu Shuoqing Zhang Xuezhang Xiao Shujiang Geng Fuhui Wang Tao Deng Lixin Chen Xiulin Fan Shenyang National Laboratory for Materials Science Northeastern UniversityShenyang 110819LiaoningChina State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province Hangzhou 310013ZhejiangChina Department of Chemical and Biomolecular Engineering University of MarylandCollege Park 20742MDUSA

Passivation by the inorganic-rich solid electrolyte interphase(sei),especially the lif-rich sei,is highly desirable to guarantee the durable lifespan of Li metal batteries(LMBs).Here,we report a diluent with the capability to facilitate the formation of lif-rich sei while avoiding the excess consumption of Li *** to most of reported inert diluents,heptafluoro-l-methoxypropane(HM) is firstly demonstrated to cooperate with the decomposition of anions to generate lif-rich sei via releasing Fcontaining species near Li *** designed electrolyte consisting of 1.8 M lifSI in the mixture of1,2-dimethoxyethane(DME)/HM(2:1 by vol.) achieves excellent compatibility with both Li metal anodes(Coulombic efficiency~99.8%) and high-voltage cathodes(4.4 V LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811) and 4.5 V LiCoO_(2)(LCO) vs Li^(+)/Li).The 4.4 V Li(20μm)‖NMC811(2.5 mA h cm^(-2)) and 4.5 V Li(20μm)‖LCO(2.5 mA h cm^(-2)) cells achieve capacity retentions of 80% over 560 cycles and 80% over 505 cycles,***,the anode-free pouch cell delivers an energy density of~293 W h kg^(-1)initially and retains 70% of capacity after 100 deep *** work highlights the critical impact of diluent on the sei formation,and opens up a new direction for designing desirable interfacial chemistries to enable high-performance LMBs.

关键词： Diluent Solvation structure lif-rich sei Li metal batteries Localized high-concentration electrolyte

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