期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 137, 期 10, 页码 3533-3539出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja5116698
关键词
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资金
- Energy Efficiency and Renewable Energy, Office of Vehicle Technologies, U.S. Department of Energy [DE-AC02-05CH11231]
- Northeastern Center for Chemical Energy Storage, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001294]
- Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-05CH11231]
Electrochemical oxidation of carbonate esters at the LixNi0.5Mn1.5O4-delta/electrolyte interface results in Ni/Mn dissolution and surface film formation, which negatively affect the electrochemical performance of Li-ion batteries. Ex situ X-ray absorption (XRF/XANES), Raman, and fluorescence spectroscopy, along with imaging of LixNi0.5Mn1.5O4-delta positive and graphite negative electrodes from tested Li-ion batteries, reveal the formation of a variety of Mn-II/III and Ni-II complexes with beta-diketonate ligands. These metal complexes, which are generated upon anodic oxidation of ethyl and diethyl carbonates at LixNi0.5Mn1.5O4-delta, form a surface film that partially dissolves in the electrolyte. The dissolved Mn-III complexes are reduced to their Mn-II analogues, which are incorporated into the solid electrolyte interphase surface layer at the graphite negative electrode. This work elucidates possible reaction pathways and evaluates their implications for Li+ transport kinetics in Li-ion batteries.
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