Abstract
A stable solid electrolyte interphase (SEI) has been proven to be a key enabler to most advanced battery chemistries, where the reactivity between the electrolyte and the anode operating beyond the electrolyte stability limits must be kinetically suppressed by such SEIs. The graphite anode used in state-of-the-art Li-ion batteries presents the most representative SEI example. Because of similar operation potentials between graphite and silicon (Si), a similar passivation mechanism has been thought to apply on the Si anode when using the same carbonate-based electrolytes. In this work, we found that the chemical formation process of a proto-SEI on Si is closely entangled with incessant SEI decomposition, detachment, and reparation, which lead to continuous lithium consumption. Using a special galvanostatic protocol designed to observe the SEI formation prior to Si lithiation, we were able to deconvolute the electrochemical formation of such dynamic SEI from the morphology and mechanical complexities of Si and showed that a pristine Si anode could not be fully passivated in carbonate-based electrolytes.
Original language | English |
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Pages (from-to) | 26593-26600 |
Number of pages | 8 |
Journal | ACS Applied Materials and Interfaces |
Volume | 12 |
Issue number | 23 |
DOIs | |
State | Published - Jun 10 2020 |
Funding
This work was authored in part by the Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under contract no. DE-AC36-08GO28308. The research is supported from the Vehicle Technologies Office of the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy under the supervision of Brian Cunningham. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes. The research is also supported by the Paul M. Rady Department of Mechanical Engineering and College of Engineering and Applied Sciences at University of Colorado Boulder. U.S. Department of Energy (DOE) under Contract no. DE-AC36-08GO28308.
Keywords
- carbonate electrolytes
- silicon anode
- solid electrolyte interphase
- surface and lithium-ion battery