Solvent-mediated oxide hydrogenation in layered cathodes

Gang Wan^{1

2}, Travis P Pollard³, Lin Ma^{3

4}, Marshall A Schroeder³, Chia-Chin Chen⁵, Zihua Zhu⁶, Zhan Zhang⁷, Cheng-Jun Sun⁷, Jiyu Cai⁸, Harry L Thaman⁹, Arturas Vailionis^{10

11}, Haoyuan Li², Shelly Kelly⁷, Zhenxing Feng¹², Joseph Franklin^{13

14}, Steven P Harvey¹⁵, Ye Zhang¹⁶, Yingge Du¹⁷, Zonghai Chen⁸, Christopher J Tassone¹, Hans-Georg Steinrück^{1

18

19

20}, Kang Xu^{3

21}, Oleg Borodin³, Michael F Toney^{1

22}

Affiliations

¹ SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
² Department of Mechanical Engineering, Stanford University, Stanford, CA 94305, USA.
³ Battery Science Branch, Energy Science Division, Army Research Directorate, DEVCOM Army Research Laboratory, Adelphi, MD 20783, USA.
⁴ Department of Mechanical Engineering and Engineering Science, The University of North Carolina at Charlotte, Charlotte, NC 28223, USA.
⁵ Department of Chemical Engineering, National Taiwan University, Taipei 10617, Taiwan.
⁶ Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99354, USA.
⁷ Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
⁸ Chemical Science and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, USA.
⁹ Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305, USA.
¹⁰ Stanford Nano Shared Facilities, Stanford University, Stanford, CA 94305, USA.
¹¹ Department of Physics, Kaunas University of Technology, LT-51368 Kaunas, Lithuania.
¹² School of Chemical, Biological, and Environmental Engineering, Oregon State University, Corvallis, OR 97331, USA.
¹³ Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
¹⁴ Department of Chemical Engineering, University College London, London WC1E 6BT, UK.
¹⁵ National Renewable Energy Laboratory, Golden, CO 80401, USA.
¹⁶ Department of Electrical and Computer Engineering and Materials Science and Engineering Program, University of Houston, Houston, TX 77204, USA.
¹⁷ Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, USA.
¹⁸ Department Chemie, Universität Paderborn, 33098 Paderborn, Germany.
¹⁹ Institute for a Sustainable Hydrogen Economy, Forschungszentrum Jülich GmbH, Marie-Curie-Straße 5, 52428 Jülich, Germany.
²⁰ RWTH Aachen University, Institute of Physical Chemistry, Landoltweg 2, 52074 Aachen, Germany.
²¹ SES AI Corporation, Woburn, MA 01801, USA.
²² Department of Chemical and Biological Engineering, Materials Science and Engineering Program, Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, CO 80309, USA.

PMID: 39265020
DOI: 10.1126/science.adg4687

Solvent-mediated oxide hydrogenation in layered cathodes

Gang Wan et al. Science. 2024.

. 2024 Sep 13;385(6714):1230-1236.

doi: 10.1126/science.adg4687. Epub 2024 Sep 12.

Authors

Affiliations

¹ SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
² Department of Mechanical Engineering, Stanford University, Stanford, CA 94305, USA.
³ Battery Science Branch, Energy Science Division, Army Research Directorate, DEVCOM Army Research Laboratory, Adelphi, MD 20783, USA.
⁴ Department of Mechanical Engineering and Engineering Science, The University of North Carolina at Charlotte, Charlotte, NC 28223, USA.
⁵ Department of Chemical Engineering, National Taiwan University, Taipei 10617, Taiwan.
⁶ Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99354, USA.
⁷ Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
⁸ Chemical Science and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, USA.
⁹ Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305, USA.
¹⁰ Stanford Nano Shared Facilities, Stanford University, Stanford, CA 94305, USA.
¹¹ Department of Physics, Kaunas University of Technology, LT-51368 Kaunas, Lithuania.
¹² School of Chemical, Biological, and Environmental Engineering, Oregon State University, Corvallis, OR 97331, USA.
¹³ Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
¹⁴ Department of Chemical Engineering, University College London, London WC1E 6BT, UK.
¹⁵ National Renewable Energy Laboratory, Golden, CO 80401, USA.
¹⁶ Department of Electrical and Computer Engineering and Materials Science and Engineering Program, University of Houston, Houston, TX 77204, USA.
¹⁷ Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, USA.
¹⁸ Department Chemie, Universität Paderborn, 33098 Paderborn, Germany.
¹⁹ Institute for a Sustainable Hydrogen Economy, Forschungszentrum Jülich GmbH, Marie-Curie-Straße 5, 52428 Jülich, Germany.
²⁰ RWTH Aachen University, Institute of Physical Chemistry, Landoltweg 2, 52074 Aachen, Germany.
²¹ SES AI Corporation, Woburn, MA 01801, USA.
²² Department of Chemical and Biological Engineering, Materials Science and Engineering Program, Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, CO 80309, USA.

PMID: 39265020
DOI: 10.1126/science.adg4687

Abstract

Self-discharge and chemically induced mechanical effects degrade calendar and cycle life in intercalation-based electrochromic and electrochemical energy storage devices. In rechargeable lithium-ion batteries, self-discharge in cathodes causes voltage and capacity loss over time. The prevailing self-discharge model centers on the diffusion of lithium ions from the electrolyte into the cathode. We demonstrate an alternative pathway, where hydrogenation of layered transition metal oxide cathodes induces self-discharge through hydrogen transfer from carbonate solvents to delithiated oxides. In self-discharged cathodes, we further observe opposing proton and lithium ion concentration gradients, which contribute to chemical and structural heterogeneities within delithiated cathodes, accelerating degradation. Hydrogenation occurring in delithiated cathodes may affect the chemo-mechanical coupling of layered cathodes as well as the calendar life of lithium-ion batteries.

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Solvent-mediated oxide hydrogenation in layered cathodes

Affiliations

Solvent-mediated oxide hydrogenation in layered cathodes

Authors

Affiliations

Abstract

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