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Concentrated ternary ether electrolyte allows for stable cycling of a lithium metal battery with commercial mass loading high-nickel NMC and thin anodes

查看全文 作　　者：Jun [1,2]Yang;Xing [1,2]Li;Ke [3,4]Qu;Yixian [5]Wang;Kangqi [6]Shen;Changhuan [4]Jiang;Bo [1,2]Yu;Pan [1,2]Luo;Zhuangzhi [1,2]Li;Mingyang [6,7]Chen;Bingshu [1,2]Guo;Mingshan [1,2]Wang;Junchen [1,2]Chen;Zhiyuan [1,2]Ma;Yun [1,2]Huang;Zhenzhong [4]Yang;Pengcheng [5]Liu;Rong [4]Huang;Xiaodi [8]Ren;David [5]Mitlin 高影响力作者 机构地区：[1]School of New Energy and Materials,Southwest Petroleum University,Chengdu,China;[2]Energy Storage Research Institute,Southwest Petroleum University,Chengdu,China;[3]Shenzhen Key Laboratory of Nanobiomechanics,Shenzhen Institutes of Advanced Technology,Chinese Academy of Sciences,Shenzhen,China;[4]China Key Laboratory of Polar Materials and Devices(MOE),Department of Electronics,East China Normal University,Shanghai,China;[5]Materials Science Program and Texas Materials Institute,The University of Texas at Austin,Austin,Texas,USA;[6]Beijing Computational Science Research Center,Beijing,China;[7]School of Materials Science and Engineering Center for Green Innovation,University of Science and Technology Beijing,Beijing,China;[8]Department of Materials Science and Engineering,Hefei National Research Center for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei,Anhui,China高影响力机构 出　　处：《Carbon Energy》索引2023年第5卷第3期,共17页高影响力期刊 基　　金：National Natural Science Foundation of China,Grant/Award Numbers:21905265,52072322,U1930402,61974042;National Science Foundation,Civil,Mechanical and Manufacturing Innovation,Grant/Award Number:1911905;Fundamental Research Funds for the Central Universities,Grant/Award Number:WK2060140026;Department of Science and Technology of Sichuan Province,Grant/Award Numbers:2019‐GH02‐00052‐HZ,2019YFG0220;Scientific and Technological Innovation Foundation of Shunde Graduate School,Grant/Award Number:BK19BE024;National Key Research and Development Program of China,Grant/Award Number:2017YFA0303403。 摘　　要：A new concentrated ternary salt ether-based electrolyte enables stable cycling of lithium metal battery(LMB)cells with high-mass-loading(13.8 mg cm^(−2),2.5 mAh cm^(−2))NMC622(LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2))cathodes and 50μm Li anodes.Termed“CETHER-3,”this electrolyte is based on LiTFSI,LiDFOB,and LiBF4 with 5 vol%fluorinated ethylene carbonate in 1,2-dimethoxyethane.Commer-cial carbonate and state-of-the-art binary salt ether electrolytes were also tested as baselines.With CETHER-3,the electrochemical performance of the full-cell battery is among the most favorably reported in terms of high-voltage cycling stability.For example,LiNi_(x)Mn_(y)Co_(1-x-y)O_(2)(NMC)-Li metal cells retain 80%capacity at 430 cycles with a 4.4 V cut-off and 83%capacity at 100 cycles with a 4.5 V cut-off(charge at C/5,discharge at C/2).According to simulation by density functional theory and molecular dynamics,this favorable performance is an outcome of enhanced coordination between Li^(+)and the solvent/salt molecules.Combining advanced microscopy(high-resolution transmission electron microscopy,scanning electron microscopy)and surface science(X-ray photoelectron spectroscopy,time-of-fight secondary ion mass spectroscopy,Fourier-transform infrared spectroscopy,Raman spectroscopy),it is demonstrated that a thinner and more stable cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)are formed.The CEI is rich in lithium sulfide(Li_(2)SO_(3)),while the SEI is rich in Li_(3)N and LiF.During cycling,the CEI/SEI suppresses both the deleterious transformation of the cathode R-3m layered near-surface structure into disordered rock salt and the growth of lithium metal dendrites. 关 键 词：concentrated electrolyte density functional theory ether electrolyte high‐nickel cathode high‐voltage battery molecular dynamics
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