Solvent-mediated oxide hydrogenation in layered cathodes

• 成果类型: Article
• 署名作者: Wan, Gang; Pollard, Travis P.; Ma, Lin; Schroeder, Marshall A.; Chen, Chia-Chin; Zhu, Zihua; Zhang, Zhan; Sun, Cheng-Jun; Cai, Jiyu; Thaman, Harry L.; Vailionis, Arturas; Li, Haoyuan; Kelly, Shelly; Feng, Zhenxing; Franklin, Joseph; Harvey, Steven P.; Zhang, Ye; Du, Yingge; Chen, Zonghai; Tassone, Christopher J.; Steinrueck, Hans-Georg; Xu, Kang; Borodin, Oleg; Toney, Michael F.
• 署名单位: Stanford University; United States Department of Energy (DOE); SLAC National Accelerator Laboratory; Stanford University; University of North Carolina; University of North Carolina Charlotte; National Taiwan University; United States Department of Energy (DOE); Pacific Northwest National Laboratory; United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Argonne National Laboratory; Stanford University; Stanford University; Kaunas University of Technology; Oregon State University; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; University of London; University College London; United States Department of Energy (DOE); National Renewable Energy Laboratory - USA; University of Houston System; University of Houston; University of Houston System; University of Houston; United States Department of Energy (DOE); Pacific Northwest National Laboratory; University of Paderborn; Helmholtz Association; Research Center Julich; RWTH Aachen University; University of Colorado System; University of Colorado Boulder
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-13221
• DOI: 10.1126/science.adg4687
• 发表日期: 2024-09-13
• 页码: 1230-1235
• 关键词: transition-metal redox; ethylene carbonate; energy-storage; lithium nickel; self-discharge; li; STABILITY; batteries; morphology; EVOLUTION

摘要

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.