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DOI10.1073/pnas.2012071118
The early-stage growth and reversibility of Li electrodeposition in Br-rich electrolytes
Biswal P.; Kludze A.; Rodrigues J.; Deng Y.; Moon T.; Stalin S.; Zhao Q.; Yin J.; Kourkoutis L.F.; Archer L.A.
发表日期2021
ISSN00278424
卷号118期号:2
英文摘要The physiochemical nature of reactive metal electrodeposits during the early stages of electrodeposition is rarely studied but known to play an important role in determining the electrochemical stability and reversibility of electrochemical cells that utilize reactive metals as anodes. We investigated the early-stage growth dynamics and reversibility of electrodeposited lithium in liquid electrolytes infused with brominated additives. On the basis of equilibrium theories, we hypothesize that by regulating the surface energetics and surface ion/adatom transport characteristics of the interphases formed on Li, Br-rich electrolytes alter the morphology of early-stage Li electrodeposits; enabling late-stage control of growth and high electrode reversibility. A combination of scanning electron microscopy (SEM), image analysis, X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), and contact angle goniometry are employed to evaluate this hypothesis by examining the physical-chemical features of the material phases formed on Li. We report that it is possible to achieve fine control of the early-stage Li electrodeposit morphology through tuning of surface energetic and ion diffusion properties of interphases formed on Li. This control is shown further to translate to better control of Li electrodeposit morphology and high electrochemical reversibility during deep cycling of the Li metal anode. Our results show that understanding and eliminating morphological and chemical instabilities in the initial stages of Li electroplating via deliberately modifying energetics of the solid electrolyte interphase (SEI) is a feasible approach in realization of deeply cyclable reactive metal batteries. © 2021 National Academy of Sciences. All rights reserved.
英文关键词Interfacial energy; Lithium metal anode; Nucleation and growth; Solid electrolyte interphase; Surface ion diffusion
语种英语
来源期刊Proceedings of the National Academy of Sciences of the United States of America
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/181042
作者单位Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, United States; Department of Materials Science and Engineering, Cornell University, Ithaca, NY 14853, United States; School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, United States; Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY 14853, United States
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Biswal P.,Kludze A.,Rodrigues J.,et al. The early-stage growth and reversibility of Li electrodeposition in Br-rich electrolytes[J],2021,118(2).
APA Biswal P..,Kludze A..,Rodrigues J..,Deng Y..,Moon T..,...&Archer L.A..(2021).The early-stage growth and reversibility of Li electrodeposition in Br-rich electrolytes.Proceedings of the National Academy of Sciences of the United States of America,118(2).
MLA Biswal P.,et al."The early-stage growth and reversibility of Li electrodeposition in Br-rich electrolytes".Proceedings of the National Academy of Sciences of the United States of America 118.2(2021).
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