Cycling Performance and Kinetic Mechanism Analysis of a Li Metal Anode in Series-Concentrated Ether Electrolytes.

Wang, S; Qu, J; Wu, F; Yan, K; Zhang, C

Cycling Performance and Kinetic Mechanism Analysis of a Li Metal Anode in Series-Concentrated Ether Electrolytes.

Wang, S Qu, J Wu, F Yan, K

Zhang, C

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Publisher:: AMER CHEMICAL SOC
Publication Type:: Journal Article
Citation:: ACS Appl Mater Interfaces, 2020, 12, (7), pp. 8366-8375
Issue Date:: 2020-02-19

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Field	Value	Language
dc.contributor.author	Wang, S
dc.contributor.author	Qu, J
dc.contributor.author	Wu, F
dc.contributor.author	Yan, K https://orcid.org/0000-0002-3623-658X
dc.contributor.author	Zhang, C
dc.date.accessioned	2021-02-05T21:24:07Z
dc.date.available	2021-02-05T21:24:07Z
dc.date.issued	2020-02-19
dc.identifier.citation	ACS Appl Mater Interfaces, 2020, 12, (7), pp. 8366-8375
dc.identifier.issn	1944-8244
dc.identifier.issn	1944-8252
dc.identifier.uri	http://hdl.handle.net/10453/145870
dc.description.abstract	Li metal batteries are facing unprecedented opportunities because of the urgent demand for high-energy-density rechargeable batteries as well as enormous challenges due to their low Coulombic efficiency and notorious safety issues. Recently, high-concentration electrolytes have attracted much attention owing to their superior properties. However, Li metal plating is an exceedingly complicated process including several elementary steps; it is not comprehensive enough to uncover the mystery of concentrated electrolytes by studying the structure of electrolytes, the existence of anions, cations, and solvent molecules using only conventional means. Here, we first report the apparent cycling performance of Li metal anode in series-concentrated LiTFSI/DOL-DME electrolytes. It shows that the Li metal anode in 4 M LiTFSI/DOL-DME electrolyte can operate 180 cycles stably at 2 mA cm-2 with an average Coulombic efficiency of 98%, in which the Li plating layer is more compact and without dendrites. Subsequently, the kinetic parameters were obtained by the microelectrode technique. We found that appropriate mass transfer, interface, and surface step kinetic parameters (migration number, exchange current density, nucleation rate, and corrosion rate) and their good matching degree are favorable for the cycling of Li metal anodes. This work reveals the relationship between the elementary steps and the apparent cycling performance during the Li plating process under certain operating conditions; it is a major breakthrough in the study of high-concentration electrolytes and can provide a new perspective for future research.
dc.language	eng
dc.publisher	AMER CHEMICAL SOC
dc.relation.ispartof	ACS Appl Mater Interfaces
dc.relation.isbasedon	10.1021/acsami.9b23251
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	03 Chemical Sciences, 09 Engineering
dc.subject.classification	Nanoscience & Nanotechnology
dc.title	Cycling Performance and Kinetic Mechanism Analysis of a Li Metal Anode in Series-Concentrated Ether Electrolytes.
dc.type	Journal Article
utslib.citation.volume	12
utslib.location.activity	United States
utslib.for	03 Chemical Sciences
utslib.for	09 Engineering
pubs.organisational-group	/University of Technology Sydney/Faculty of Science
pubs.organisational-group	/University of Technology Sydney
utslib.copyright.status	closed_access	*
dc.date.updated	2021-02-05T21:23:41Z
pubs.issue	7
pubs.publication-status	Published
pubs.volume	12
utslib.citation.issue	7

Abstract:

Li metal batteries are facing unprecedented opportunities because of the urgent demand for high-energy-density rechargeable batteries as well as enormous challenges due to their low Coulombic efficiency and notorious safety issues. Recently, high-concentration electrolytes have attracted much attention owing to their superior properties. However, Li metal plating is an exceedingly complicated process including several elementary steps; it is not comprehensive enough to uncover the mystery of concentrated electrolytes by studying the structure of electrolytes, the existence of anions, cations, and solvent molecules using only conventional means. Here, we first report the apparent cycling performance of Li metal anode in series-concentrated LiTFSI/DOL-DME electrolytes. It shows that the Li metal anode in 4 M LiTFSI/DOL-DME electrolyte can operate 180 cycles stably at 2 mA cm-2 with an average Coulombic efficiency of 98%, in which the Li plating layer is more compact and without dendrites. Subsequently, the kinetic parameters were obtained by the microelectrode technique. We found that appropriate mass transfer, interface, and surface step kinetic parameters (migration number, exchange current density, nucleation rate, and corrosion rate) and their good matching degree are favorable for the cycling of Li metal anodes. This work reveals the relationship between the elementary steps and the apparent cycling performance during the Li plating process under certain operating conditions; it is a major breakthrough in the study of high-concentration electrolytes and can provide a new perspective for future research.

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http://hdl.handle.net/10453/145870