title: Phase evolution for conversion reaction electrodes in lithium-ion batteries.
abstract: The performance of battery materials is largely governed by structural and chemical evolutions during electrochemical reactions. Therefore, resolving spatially dependent reaction pathways could enlighten mechanistic understanding, and enable rational design for rechargeable battery materials. Here, we present a phase evolution panorama via spectroscopic and three-dimensional imaging at multiple states of charge for an anode material (that is, nickel oxide nanosheets) in lithium-ion batteries. We reconstruct the three-dimensional lithiation/delithiation fronts and find that, in a fully electrolyte immersion environment, phase conversion can nucleate from spatially distant locations on the same slab of material. In addition, the architecture of a lithiated nickel oxide is a bent porous metallic framework. Furthermore, anode-electrolyte interphase is found to be dynamically evolving upon charging and discharging. The present study has implications for resolving the inhomogeneity of the general electrochemically driven phase transition (for example, intercalation reactions) and for the origin of inhomogeneous charge distribution in large-format battery electrodes.
authors.affiliation: 1] Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA [2] Department of Chemistry and Geochemistry, Materials Science Program, Colorado School of Mines, Golden, Colorado 80401, USA.
authors.forename: Feng
authors.initials: F
authors.lastname: Lin
authors.affiliation: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors.forename: Dennis
authors.initials: D
authors.lastname: Nordlund
authors.affiliation: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors.forename: Tsu-Chien
authors.initials: TC
authors.lastname: Weng
authors.affiliation: 1] Monash Centre for Electron Microscopy, Monash University, Victoria 3800, Australia [2] Department of Materials Engineering, Monash University, Victoria 3800, Australia.
authors.forename: Ye
authors.initials: Y
authors.lastname: Zhu
authors.affiliation: Chemical and Materials Science Center, National Renewable Energy Laboratory, Golden, Colorado 80401, USA.
authors.forename: Chunmei
authors.initials: C
authors.lastname: Ban
authors.affiliation: Department of Chemistry and Geochemistry, Materials Science Program, Colorado School of Mines, Golden, Colorado 80401, USA.
authors.forename: Ryan M
authors.initials: RM
authors.lastname: Richards
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: Huolin L
authors.initials: HL
authors.lastname: Xin