Activated Internetwork Pathways in Partially‐Disordered Spinel Cathode Materials with Ultrahigh Rate Performance

Yang, Julia H.; Ceder, Gerbrand

doi:10.1002/aenm.202202955

Activated Internetwork Pathways in Partially‐Disordered Spinel Cathode Materials with Ultrahigh Rate Performance

Journal Article · Fri Dec 09 04:00:00 EST 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202202955· OSTI ID:1922518

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Department of Materials Science and Engineering University of California Berkeley CA 94720 USA, Materials Science Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA

Abstract

In this study, a class of earth‐abundant, cation‐excess partially disordered spinel materials which demonstrate superior rate performance as Li‐ion cathodes compared to disordered rocksalt materials is computationally investigated. These results show that the partial disorder creates solid solution lithiation with spinel‐like features at the atomic level. A low‐voltage capacity gain is possible with lithiation past the rock salt stoichiometry. It is argued that high rate in partially disordered spinel materials comes from newly activated 16c/16d internetwork pathways which are not possible in normal spinel where only 16c intranetwork diffusion occurs. The assessment and understandings motivate the incorporation of some degree of partial spinel ordering in future disordered rocksalt electrodes to enable superior rate performance.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; AC02-05CH11231

OSTI ID:: 1922518

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 4 Vol. 13; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (21)

The Configurational Space of Rocksalt-Type Oxides for High-Capacity Lithium Battery Electrodes Urban, Alexander; Lee, Jinhyuk; Ceder, Gerbrand Advanced Energy Materials, Vol. 4, Issue 13 https://doi.org/10.1002/aenm.201400478	journal	May 2014
Disordered Lithium-Rich Oxyfluoride as a Stable Host for Enhanced Li ⁺ Intercalation Storage Chen, Ruiyong; Ren, Shuhua; Knapp, Michael Advanced Energy Materials, Vol. 5, Issue 9 https://doi.org/10.1002/aenm.201401814	journal	February 2015
Die Berechnung optischer und elektrostatischer Gitterpotentiale Ewald, P. P. Annalen der Physik, Vol. 369, Issue 3 https://doi.org/10.1002/andp.19213690304	journal	January 1921
Generalized cluster description of multicomponent systems Sanchez, J. M.; Ducastelle, F.; Gratias, D. Physica A: Statistical Mechanics and its Applications, Vol. 128, Issue 1-2 https://doi.org/10.1016/0378-4371(84)90096-7	journal	November 1984
Multicomponent multisublattice alloys, nonconfigurational entropy and other additions to the Alloy Theoretic Automated Toolkit van de Walle, Axel Calphad, Vol. 33, Issue 2 https://doi.org/10.1016/j.calphad.2008.12.005	journal	June 2009
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav Computational Materials Science, Vol. 68 https://doi.org/10.1016/j.commatsci.2012.10.028	journal	February 2013
Toward high-energy Mn-based disordered-rocksalt Li-ion cathodes Li, Hao; Fong, Richie; Woo, Moohyun Joule, Vol. 6, Issue 1 https://doi.org/10.1016/j.joule.2021.11.005	journal	January 2022
Factors affecting Li mobility in spinel LiMn2O4—A first-principles study by GGA and GGA+U methods Xu, Bo; Meng, Shirley Journal of Power Sources, Vol. 195, Issue 15 https://doi.org/10.1016/j.jpowsour.2010.02.060	journal	August 2010
Realizing continuous cation order-to-disorder tuning in a class of high-energy spinel-type Li-ion cathodes Cai, Zijian; Ji, Huiwen; Ha, Yang Matter, Vol. 4, Issue 12 https://doi.org/10.1016/j.matt.2021.10.013	journal	December 2021
Role of Electronic Structure in the Susceptibility of Metastable Transition-Metal Oxide Structures to Transformation Reed, John; Ceder, Gerbrand Chemical Reviews, Vol. 104, Issue 10 https://doi.org/10.1021/cr020733x	journal	October 2004
Computational understanding of Li-ion batteries Urban, Alexander; Seo, Dong-Hwa; Ceder, Gerbrand npj Computational Materials, Vol. 2, Issue 1 https://doi.org/10.1038/npjcompumats.2016.2	journal	March 2016
Hidden structural and chemical order controls lithium transport in cation-disordered oxides for rechargeable batteries Ji, Huiwen; Urban, Alexander; Kitchaev, Daniil A. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08490-w	journal	February 2019
A reflection on lithium-ion battery cathode chemistry Manthiram, Arumugam Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15355-0	journal	March 2020
Approaches for handling high-dimensional cluster expansions of ionic systems Yang, Julia H.; Chen, Tina; Barroso-Luque, Luis npj Computational Materials, Vol. 8, Issue 1 https://doi.org/10.1038/s41524-022-00818-3	journal	June 2022
Ultrahigh power and energy density in partially ordered lithium-ion cathode materials Ji, Huiwen; Wu, Jinpeng; Cai, Zijian Nature Energy, Vol. 5, Issue 3 https://doi.org/10.1038/s41560-020-0573-1	journal	March 2020
Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries Lun, Zhengyan; Ouyang, Bin; Kwon, Deok-Hwang Nature Materials, Vol. 20, Issue 2 https://doi.org/10.1038/s41563-020-00816-0	journal	October 2020
Cation-disordered rocksalt transition metal oxides and oxyfluorides for high energy lithium-ion cathodes Clément, R. J.; Lun, Z.; Ceder, G. Energy & Environmental Science, Vol. 13, Issue 2 https://doi.org/10.1039/C9EE02803J	journal	January 2020
Effect of fluorination and Li-excess on the Li migration barrier in Mn-based cathode materials Jadidi, Zinab; Chen, Tina; Xiao, Penghao Journal of Materials Chemistry A, Vol. 8, Issue 38 https://doi.org/10.1039/D0TA06415G	journal	January 2020
Model for Configurational Thermodynamics in Ionic Systems Tepesch, P. D.; Garbulsky, G. D.; Ceder, G. Physical Review Letters, Vol. 74, Issue 12 https://doi.org/10.1103/PhysRevLett.74.2272	journal	March 1995
Structure of Spinel Sickafus, Kurt E.; Wills, John M.; Grimes, Norman W. Journal of the American Ceramic Society, Vol. 82, Issue 12 https://doi.org/10.1111/j.1151-2916.1999.tb02241.x	journal	December 1999
Unlocking the Potential of Cation-Disordered Oxides for Rechargeable Lithium Batteries Lee, J.; Urban, A.; Li, X. Science, Vol. 343, Issue 6170 https://doi.org/10.1126/science.1246432	journal	January 2014

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