Journal article
How Transition Metals Enable Electron Transfer through the SEI: Part II. Redox-Cycling Mechanism Model and Experiment
Journal of the Electrochemical Society, v 167(1), p13503
26 Aug 2019
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
At high operating voltages, metals like Mn, Ni, and Co dissolve from Li-ion cathodes, deposit at the anode, and interfere with the performance of the solid-electrolyte interphase (SEI) to cause constant Li loss. The mechanism by which these metals disrupt SEI processes at the anode remains poorly understood. Experiments from Part I of this work demonstrate that Mn, Ni, and Co all affect the electronic properties of the SEI much more than the morphology, and that Mn is the most aggressively disruptive of the three metals. In this work we determine how a proposed electrocatalytic mechanism can explain why Mn contamination is uniquely detrimental to SEI passivation. We develop a microkinetic model of the redox cycling mechanism and apply it to experiments from Part I. The results show that the thermodynamicmetal reduction potential does not explain why Mn is the most active of the three metals. Instead, kinetic differences between the three metals are more likely to govern their reactivity in the SEI. Our results emphasize the importance of local coordination environment and proximity to the anode within the SEI for controlling electron transfer and resulting capacity fade. (C) The Author(s) 2019. Published by ECS.
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Details
- Title
- How Transition Metals Enable Electron Transfer through the SEI: Part II. Redox-Cycling Mechanism Model and Experiment
- Creators
- Oliver C. Harris - Drexel UniversityKevin Leung - Sandia National Laboratories CaliforniaMaureen H. Tang - Drexel UniversitySandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Publication Details
- Journal of the Electrochemical Society, v 167(1), p13503
- Publisher
- Electrochemical Soc Inc
- Number of pages
- 8
- Grant note
- DE-NA0003525 / U.S. Department of Energy's National Nuclear Security Administration; National Nuclear Security Administration 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)
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemical and Biological Engineering
- Web of Science ID
- WOS:000483946600002
- Scopus ID
- 2-s2.0-85077151504
- Other Identifier
- 991019168704804721
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Electrochemistry
- Materials Science, Coatings & Films