Journal article
How Transition Metals Enable Electron Transfer through the SEI: Part I. Experiments and Butler-Volmer Modeling
Journal of the Electrochemical Society, v 167(1), p13502
26 Aug 2019
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
Transition metal dissolution from high-voltage Li-ion battery cathodes disrupts the formation and performance of the solid-electrolyte interphase (SEI). SEI contamination by transition metals results in continual Li loss and severe capacity fade. Fundamental understanding of how metals undermine SEI passivation is necessary to mitigate this degradation. This two-part study interrogates the mechanisms by which transition metals facilitate through-film charge-transfer and SEI failure. Part I presents experimental results in which we intentionally contaminate SEIs with Mn, Ni, and Co. Rotating disk electrode voltammetry of a redox mediator quantifies how each metal impacts the charge-transfer characteristics of the SEI. A physics-based model finds that all three metals disrupt the electronic properties of the SEI more than the morphology. Surprisingly, the Butler-Volmer kinetics of charge-transfer through a Mn-contaminated SEI are an order of magnitude faster than for a Co-contaminated SEI, even with similar embeddedmetal concentrations. Such trends between metals are inconsistent with bandgap predictions from density functional theory, implying an alternative redox-cycling mechanism, which is mathematically developed and compared to experiment in Part II. (C) The Author(s) 2019. Published by ECS.
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Details
- Title
- How Transition Metals Enable Electron Transfer through the SEI: Part I. Experiments and Butler-Volmer Modeling
- Creators
- Oliver C. Harris - Drexel UniversityYuxiao Lin - Michigan State UniversityYue Qi - Michigan State UniversityKevin Leung - Sandia National Laboratories CaliforniaMaureen H. Tang - Drexel UniversityUniv. of Maryland, College Park, MD (United States)
- Publication Details
- Journal of the Electrochemical Society, v 167(1), p13502
- Publisher
- Electrochemical Soc Inc
- Number of pages
- 9
- Grant note
- DESC0001160 / Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; United States Department of Energy (DOE) DMR1832808 / National Science Foundation; National Science Foundation (NSF) DE-NA0003525 / U. S. Department of Energy's National Nuclear Security Administration; National Nuclear Security Administration
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemical and Biological Engineering
- Web of Science ID
- WOS:000483946600001
- Scopus ID
- 2-s2.0-85077149707
- Other Identifier
- 991019168787104721
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Electrochemistry
- Materials Science, Coatings & Films