Revealing the Chemical and Structural Complexity of Electrochemical Ion Exchange in Layered Oxide Materials.

Autor: Mu L; Department of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United States.; School for Engineering of Matter, Transport and Energy, Arizona State University, Tempe, Arizona 85287, United States., Hou D; Department of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United States.; Institute for Materials Research and Innovation (IMRI), University of Louisiana at Lafayette, Lafayette, Louisiana 70503, United States., Foley EE; Materials Department and Materials Research Laboratory, University of California Santa Barbara, Santa Barbara, California 93106, United States., Dai M; Department of Materials Science and Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States., Zhang J; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Jiang Z; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Rahman MM; Department of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United States., Fu Y; Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Ma L; National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, United States., Hu E; Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States., Sainio S; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Nordlund D; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Liu J; Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States., Hu JM; Department of Materials Science and Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States., Liu Y; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Clément RJ; Materials Department and Materials Research Laboratory, University of California Santa Barbara, Santa Barbara, California 93106, United States., Lin F; Department of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United States.; Department of Materials Science and Engineering, Virginia Tech, Blacksburg, Virginia 24061, United States.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2024 Oct 02; Vol. 146 (39), pp. 26916-26925. Date of Electronic Publication: 2024 Sep 17.
DOI: 10.1021/jacs.4c08089
Abstrakt: Soft chemistry techniques, such as ion exchange, hold great potential for the development of battery electrode materials that cannot be stabilized via conventional equilibrium synthesis methods. Nevertheless, the intricate mechanisms governing ion exchange remain elusive. Herein, we investigate the evolution of the long-range and local structure, as well as the ion (de)intercalation mechanism during electrochemical Li-to-Na ion exchange initiated from an O3-type lithium-layered oxide cathode. The in situ -formed mixed-cation electrolyte leads to competitive intercalation of Li and Na ions. While Li ion intercalation predominates at the beginning of initial discharge, Na ion cointercalation into a different layer results in ion redistribution and phase separation, with the emergence of a P3-Na phase alongside an O3-Li phase. Further, this study spatially resolves the heterogeneous nature of electrochemical ion exchange reactions within individual particles and provides insights into the correlations between local Ni redox processes and phase separation. Overall, electrochemical ion exchange leads to a mixed-phase cathode and alters its reaction kinetics. Those findings have important implications for the development of new metastable materials for renewable energy devices and ion separation applications.
Databáze: MEDLINE
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