University of Oulu

Zhang, Y., Hu, A., Liu, J., Xu, Z., Mu, L., Sainio, S., Nordlund, D., Li, L., Sun, C.-J., Xiao, X., Liu, Y., Lin, F., Investigating Particle Size-Dependent Redox Kinetics and Charge Distribution in Disordered Rocksalt Cathodes. Adv. Funct. Mater. 2022, 32, 2110502.

Investigating particle size-dependent redox kinetics and charge distribution in disordered rocksalt cathodes

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Author: Zhang, Yuxin1; Hu, Anyang1; Liu, Jue2;
Organizations: 1Department of Chemistry, Virginia Tech, Blacksburg, VA, 24073 USA
2Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831 USA
3Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025 USA
4Microelectronics Research Unit, Faculty of Information Technology and Electrical Engineering, Univeristy of Oulu, Oulu, 90570 Finland
5Advanced Photon Source, Argonne National Laboratory, Lemont, IL, 60439 USA
6National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, 11973 USA
Format: article
Version: published version
Access: open
Online Access: PDF Full Text (PDF, 4.1 MB)
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Language: English
Published: John Wiley & Sons, 2022
Publish Date: 2022-07-19


Understanding how various redox activities evolve and distribute in disordered rocksalt oxides (DRX) can advance insights into manipulating materials properties for achieving stable, high-energy batteries. Herein, the authors present how the reaction kinetics and spatial distribution of redox activities are governed by the particle size of DRX materials. The size-dependent electrochemical performance is attributed to the distinct cationic and anionic reaction kinetics at different sizes, which can be tailored to achieve optimal capacity and stability. Overall, the local charged domains in DRX particles display random heterogeneity caused by the isotropic delithiation pathways. Owing to the kinetic limitation, the micron-sized particles exhibit a holistic “core-shell” charge distribution, whereas sub-micron particles show more uniform redox reactions throughout the particles and ensembles. Sub-micron DRX particles exhibit increasing anionic redox activities yet inferior cycling stability. In summary, engineering particle size can effectively modulate how cationic and anionic redox activities evolve and distribute in DRX materials.

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Series: Advanced functional materials
ISSN: 1616-301X
ISSN-E: 1616-3028
ISSN-L: 1616-301X
Volume: 32
Issue: 17
Article number: 2110502
DOI: 10.1002/adfm.202110502
Type of Publication: A1 Journal article – refereed
Field of Science: 216 Materials engineering
114 Physical sciences
Funding: The work was supported by the Thomas F. and Kate Miller Jeffress Memorial Trust, Bank of America, Trustee and the Jeffress Trust Awards Program in Interdisciplinary Research, and the National Science Foundation (DMR-2045570). Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. This research the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Research conducted at Spallation Neutron Source in Oak Ridge National Laboratory (NOMAD) was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. S.S. has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 841621. S.S. acknowledges funding from the Walter Ahlström Foundation.
EU Grant Number: (841621) TACOMA - Towards Application specific tailoring of CarbOn nanoMAterials
Copyright information: © 2022 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution-NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.