Journal
NANO LETTERS
Volume 15, Issue 9, Pages 6170-6176Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.5b02479
Keywords
In situ liquid SIMS; solid-liquid interface; molecular structural evolution; lithium ion battery; SEI layers
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Funding
- Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - Department of Energy, Office of Science, Basic Energy Sciences
- Office of Vehicle Technologies of the U.S. Department of Energy [DE-AC02-05CH11231, 6951379]
- U.S. Department of Energy (DOE) [DE-AC05- 76RL01830]
- Department of Energy's Office of Biological and Environmental Research
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Dynamic structural and chemical evolution at solid-liquid electrolyte interface is always a mystery for a rechargeable battery due to the challenge to directly probe a solid-liquid interface under reaction conditions. We describe the creation and usage of in situ liquid secondary ion mass spectroscopy (SIMS) for the first time to directly observe the molecular structural evolution at the solid-liquid electrolyte interface for a lithium (Li)-ion battery under dynamic operating conditions. We have discovered that the deposition of Li metal on copper electrode leads to the condensation of solvent molecules around the electrode. Chemically, this layer of solvent condensate tends to be depleted of the salt anions and with reduced concentration of Li+ ions, essentially leading to the formation of a lean electrolyte layer adjacent to the electrode and therefore contributing to the overpotential of the cell. This observation provides unprecedented molecular level dynamic information on the initial formation of the solid electrolyte interphase (SEI) layer. The present work also ultimately opens new avenues for implanting the in situ liquid SIN'S concept to probe the chemical reaction process that intimately involves solid-liquid interface, such as electrocatalysis, electrodeposition, biofuel conversion, biofilm, and biomineralization.
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