Beyond Constant Current: Origin of Pulse-Induced Activation in Phase-Transforming Battery ElectrodesClick to copy article linkArticle link copied!
- Haitao D. DengHaitao D. DengDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesMore by Haitao D. Deng
- Norman JinNorman JinDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesMore by Norman Jin
- Peter M. AttiaPeter M. AttiaDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesMore by Peter M. Attia
- Kipil LimKipil LimDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesStanford Institute for Materials & Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United StatesMore by Kipil Lim
- Stephen D. KangStephen D. KangDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesMore by Stephen D. Kang
- Nidhi KapateNidhi KapateDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesMore by Nidhi Kapate
- Hongbo ZhaoHongbo ZhaoDepartment of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United StatesMore by Hongbo Zhao
- Yiyang LiYiyang LiDepartment of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesMore by Yiyang Li
- Martin Z. BazantMartin Z. BazantDepartment of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United StatesDepartment of Mathematics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United StatesMore by Martin Z. Bazant
- William C. Chueh*William C. Chueh*Email: [email protected]Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United StatesStanford Institute for Materials & Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United StatesMore by William C. Chueh
Abstract
Mechanistic understanding of phase transformation dynamics during battery charging and discharging is crucial toward rationally improving intercalation electrodes. Most studies focus on constant-current conditions. However, in real battery operation, such as in electric vehicles during discharge, the current is rarely constant. In this work we study current pulsing in LiXFePO4 (LFP), a model and technologically important phase-transforming electrode. A current-pulse activation effect has been observed in LFP, which decreases the overpotential by up to ∼70% after a short, high-rate pulse. This effect persists for hours or even days. Using scanning transmission X-ray microscopy and operando X-ray diffraction, we link this long-lived activation effect to a pulse-induced electrode homogenization on both the intra- and interparticle length scales, i.e., within and between particles. Many-particle phase-field simulations explain how such pulse-induced homogeneity contributes to the decreased electrode overpotential. Specifically, we correlate the extent and duration of this activation to lithium surface diffusivity and the magnitude of the current pulse. This work directly links the transient electrode-level electrochemistry to the underlying phase transformation and explains the critical effect of current pulses on phase separation, with significant implication on both battery round-trip efficiency and cycle life. More broadly, the mechanisms revealed here likely extend to other phase-separating electrodes, such as graphite.
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This article is cited by 3 publications.
- Mingzhe Leng, Changhua Hu, Zhijie Zhou, Chi Xia, Leqiong Xie, Xuemei Li, Zhaoqiang Wang, Chuanyang Li, Li Wang, Yating Chang, Zhanrong Zhou, Xiangming He. Advanced pulse charging strategies enhancing performances of lithium-ion battery: Fundamentals, advances and outlooks. eTransportation 2025, 24 , 100402. https://doi.org/10.1016/j.etran.2025.100402
- Alexis Geslin, Le Xu, Devi Ganapathi, Kevin Moy, William C. Chueh, Simona Onori. Dynamic cycling enhances battery lifetime. Nature Energy 2024, 4 https://doi.org/10.1038/s41560-024-01675-8
- Tushar K. Telmasre, Anthony César Concepción, Suryanarayana Kolluri, Lubhani Mishra, Raghav S. Thiagarajan, Aditya Naveen Matam, Akshay Subramaniam, Taylor R. Garrick, Venkat R. Subramanian. Perspective—Moving Next-Generation Phase-Field Models to BMS Applications: A Case Study that Confirms Professor Uzi Landau’s Foresight. Journal of The Electrochemical Society 2024, 171
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, 063507. https://doi.org/10.1149/1945-7111/ad57f9
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