Revealing the Chemical and Structural Complexity of Electrochemical Ion Exchange in Layered Oxide Materials
Year: 2024
Type: article
Abstract: High Resolution Image Download MS PowerPoint Slide 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.
DOI: 10.1021/jacs.4c08089
Institutions: Arizona State University, Virginia Tech, University of Louisiana at Lafayette, University of California, Santa Barbara, University of Wisconsin–Madison, SLAC National Accelerator Laboratory, Stanford Synchrotron Radiation Lightsource, Lawrence Berkeley National Laboratory, Brookhaven National Laboratory, National Synchrotron Light Source II, Oak Ridge National Laboratory
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,500
Funders: National Science Foundation, U.S. Department of Energy, Arizona State University, Office of Science, American Chemical Society Petroleum Research Fund, University of California, Santa Barbara, Materials Research Science and Engineering Center, Harvard University, Division of Materials Research, Office of Advanced Cyberinfrastructure, Division of Chemical, Bioengineering, Environmental, and Transport Systems, Basic Energy Sciences, Argonne National Laboratory, Oak Ridge National Laboratory, Brookhaven National Laboratory, SLAC National Accelerator Laboratory, National Science Foundation Graduate Research Fellowship Program
Awards: G1003364744, G1015391036, G1141670404, G1229526393, G1285306620, G1286251239, G1313983767, G1439220948, G1453181110, G171842289, G1847291448, G1859982448, Track 4: Advanced CI Coordination Ecosystem: Monitoring and Measurement Services, Magnetic-field Control of Ionic Bonds on Polar Surfaces by Design, G2027916244, G2232042528, G2371548206, G241279073, G2569087844, G2591139515, G262532246, G2692744044, G2699395039, G2817899265, G2885514473, G299465554, G303061748, Materials Research Science and Engineering Center at UCSB, G3228777763, G3262563802, G3265821332, G3406661761, G3526003852, G3562386289, G357145406, G3809228459, G3898241218, G3927959030, G3993056153, Track 1: ACCESS Resource Allocations Marketplace and Platform Services (RAMPS), G4010157413, G401861217, G4235786860, G4281768896, G4471177777, G4478963120, G4590128248, G4654690619, ACO: An Open CI Ecosystem to Advance Scientific Discovery (OpenCI), G486153830, G4908923434, G495301720, G498139845, Track 3: COre National Ecosystem for CyberinfrasTructure (CONECT), G5098925467, G5212984984, G5237682622, G5367127336, G5464919783, CAREER: High-Resolution NMR for Paramagnetic Sodium Electrodes, G5570207115, G5602398950, G5704573845, G5765906131, G6025207788, G6121277264, G618388848, G6247045938, G6282714480, G628751139, G6456098427, G6473820372, G6550344761, G6671297155, G6801133143, Graduate Research Fellowship Program (GRFP), G6965541988, G6965887028, G7007321473, G7083997402, G7283024673, G7313278570, Collaborative Research: Chemomechanical Degradation of Oxide Cathodes in Li-ion Batteries: Synchrotron Analysis, Environmental Measurements, and Data Mining, Direct Observation of Protein Self-Assembly with Liquid-Phase Transmission Electron Microscopy, G7463374569, G7518380869, G754761654, G7600907426, G7872514369, Collaborative Research: Probing and Tailoring the Cathode-Electrolyte Interfacial Chemistries for Sodium Ion Batteries, G8174472116, Track 2: Customized Multi-tier Assistance, Training, and Computational Help (MATCH) for End User ACCESS to CI, G8382000481, G872144517, G8801403457, G8950789811, G911061179, G969889393
OpenAlex ID: W4402555911