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Promoting Reversibility of Multielectron Redox in Alkali-Rich Sulfide Cathodes through Cryomilling

Kim, Seong Shik and Agyeman-Budu, David N. and Zak, Joshua J. and Dawson, Andrew and Yan, Qizhang and Cabán-Acevedo, Miguel and Wiaderek, Kamila M. and Yakovenko, Andrey A. and Yao, Yiyi and Irshad, Ahamed and Narayan, Sri R. and Luo, Jian and Nelson Weker, Johanna and Tolbert, Sarah H. and See, Kimberly A. (2022) Promoting Reversibility of Multielectron Redox in Alkali-Rich Sulfide Cathodes through Cryomilling. Chemistry of Materials, 34 (7). pp. 3236-3245. ISSN 0897-4756. doi:10.1021/acs.chemmater.2c00030. https://resolver.caltech.edu/CaltechAUTHORS:20220318-695727237

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Abstract

Conventional cathodes for Li-ion batteries (LIBs) are reaching their theoretical capacity limits. One way to meet the growing demands for high-capacity LIBs is by developing so-called Li-rich cathode materials that greatly benefit from additional capacities from anionic moieties in the structure. Li-rich materials are intrinsically subject to higher degrees of (de)intercalation, leaving the particles more prone to fractures and thus rapid capacity fade. Alkali-rich LiNaFeS₂ reversibly cycles with capacities exceeding 300 mAh g⁻¹, but its capacity fades faster than an isostructural material Li₂FeS₂. Using synchrotron-based transmission X-ray microscopy (TXM), we demonstrate that the capacity fade of LiNaFeS₂ stems from particle fractures in the first charge cycle. We improve the cycling performance of LiNaFeS₂ by means of cryomilling, which enhances capacity retention at cycle 50 by 76%. Through crystallographic and morphological characterization techniques, we confirm that cryomilling not only decreases particle and crystallite size while increasing microstrain but also prevents particles from fracturing. Cryomilling is a powerful tool to engineer nanoscale battery materials, and TXM allows the direct observation of morphological changes of the particles, which can be leveraged to develop next-generation cathode materials for LIBs.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.chemmater.2c00030DOIArticle
ORCID:
AuthorORCID
Kim, Seong Shik0000-0003-2604-6392
Agyeman-Budu, David N.0000-0002-3461-8373
Zak, Joshua J.0000-0003-3793-7254
Yan, Qizhang0000-0002-3798-642X
Cabán-Acevedo, Miguel0000-0003-0054-8044
Wiaderek, Kamila M.0000-0002-0051-3661
Irshad, Ahamed0000-0001-7107-9623
Narayan, Sri R.0000-0002-7259-3728
Luo, Jian0000-0002-5424-0216
Nelson Weker, Johanna0000-0001-6856-3203
Tolbert, Sarah H.0000-0001-9969-1582
See, Kimberly A.0000-0002-0133-9693
Additional Information:© 2022 American Chemical Society. Received: January 4, 2022; Revised: February 28, 2022; Published: March 17, 2022. This work was supported as part of the Center for Synthetic Control Across Length-scales for Advancing Rechargeables (SCALAR), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0019381. J.J.Z. acknowledges support from the National Science Foundation Graduate Research Fellowship under Grant. No. DGE-1745301. 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. S.S.K. and M.C.-A. acknowledge the Kavli Nanoscience Institute at Caltech for TEM infrastructure and support. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The authors declare no competing financial interest.
Group:Kavli Nanoscience Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0019381
NSF Graduate Research FellowshipDGE-1745301
Department of Energy (DOE)DE-AC02-76SF00515
Department of Energy (DOE)DE-AC02-06CH11357
Subject Keywords:Nanoparticles, Electrodes, Deformation, Diffraction, Materials
Issue or Number:7
DOI:10.1021/acs.chemmater.2c00030
Record Number:CaltechAUTHORS:20220318-695727237
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20220318-695727237
Official Citation:Promoting Reversibility of Multielectron Redox in Alkali-Rich Sulfide Cathodes through Cryomilling. Seong Shik Kim, David N. Agyeman-Budu, Joshua J. Zak, Andrew Dawson, Qizhang Yan, Miguel Cában-Acevedo, Kamila M. Wiaderek, Andrey A. Yakovenko, Yiyi Yao, Ahamed Irshad, Sri R. Narayan, Jian Luo, Johanna Nelson Weker, Sarah H. Tolbert, and Kimberly A. See. Chemistry of Materials 2022 34 (7), 3236-3245; DOI: 10.1021/acs.chemmater.2c00030
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:113963
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:18 Mar 2022 14:20
Last Modified:15 Jul 2022 16:36

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  • Kim, Seong Shik and Agyeman-Budu, David N. and Zak, Joshua J. and Dawson, Andrew and Yan, Qizhang and Cabán-Acevedo, Miguel and Wiaderek, Kamila M. and Yakovenko, Andrey A. and Yao, Yiyi and Irshad, Ahamed and Narayan, Sri R. and Luo, Jian and Nelson Weker, Johanna and Tolbert, Sarah H. and See, Kimberly A. Promoting Reversibility of Multielectron Redox in Alkali-Rich Sulfide Cathodes through Cryomilling. (deposited 18 Mar 2022 14:20) [Currently Displayed]

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