Solvent-mediated oxide hydrogenation in layered cathodes
Journal
Science (New York, N.Y.)
Journal Volume
385
Journal Issue
6714
Start Page
1230
End Page
1236
ISSN
0036-8075
1095-9203
Date Issued
2024-09-13
Author(s)
Gang Wan
Travis P. Pollard
Lin Ma
Marshall A. Schroeder
Zihua Zhu
Zhan Zhang
Cheng-Jun Sun
Jiyu Cai
Harry L. Thaman
Arturas Vailionis
Haoyuan Li
Shelly Kelly
Zhenxing Feng
Joseph Franklin
Steven P. Harvey
Ye Zhang
Yingge Du
Zonghai Chen
Christopher J. Tassone
Hans-Georg Steinrück
Kang Xu
Oleg Borodin
Michael F. Toney
DOI
10.1126/science.adg4687
Abstract
Self-discharge and chemically induced mechanical effects degrade calendar and cycle life in intercalation-based electrochromic and electrochemical energy storage devices. In rechargeable lithium-ion batteries, self-discharge in cathodes causes voltage and capacity loss over time. The prevailing self-discharge model centers on the diffusion of lithium ions from the electrolyte into the cathode. We demonstrate an alternative pathway, where hydrogenation of layered transition metal oxide cathodes induces self-discharge through hydrogen transfer from carbonate solvents to delithiated oxides. In self-discharged cathodes, we further observe opposing proton and lithium ion concentration gradients, which contribute to chemical and structural heterogeneities within delithiated cathodes, accelerating degradation. Hydrogenation occurring in delithiated cathodes may affect the chemo-mechanical coupling of layered cathodes as well as the calendar life of lithium-ion batteries.
Publisher
American Association for the Advancement of Science (AAAS)
Type
journal article