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Enhancing the Electrode Gravimetric Capacity of Li1.2Mn0.4Ti0.4O2 Cathode Using Interfacial Carbon Deposition and Carbon Nanotube-Mediated Electrical Percolation

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    Functional Nanostructured Materials (including low-D carbon)

    Enhancing the Electrode Gravimetric Capacity of Li1.2Mn0.4Ti0.4O2 Cathode Using Interfacial Carbon Deposition and Carbon Nanotube-Mediated Electrical Percolation
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    • Jianan Xu
      Jianan Xu
      Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States
      More by Jianan Xu
    • Shripad Patil
      Shripad Patil
      Bredesen Center for Interdisciplinary Research and Education, University of Tennessee Knoxville, Knoxville, Tennessee 37996, United States
      Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States
      More by Shripad Patil
    • Krishna Prasad Koirala
      Krishna Prasad Koirala
      Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
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    • Weiyin Chen
      Weiyin Chen
      Department of Chemistry, Rice University, Houston, Texas 77005, United States
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      Orcidhttps://orcid.org/0000-0002-6427-4129
    • Astrid Campos-Mata
      Astrid Campos-Mata
      Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States
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    • Chongmin Wang
      Chongmin Wang
      Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
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      Orcidhttps://orcid.org/0000-0003-3327-0958
    • Soumyabrata Roy*
      Soumyabrata Roy
      Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0003-3540-1341
    • Jagjit Nanda*
      Jagjit Nanda
      Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States
      Applied Energy Division SLAC National Laboratory 2575, Sand Hill Road, Menlo Park, California 94025, United States
      *Email: [email protected]
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    • Pulickel M. Ajayan*
      Pulickel M. Ajayan
      Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-8323-7860
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 26, 31711–31719
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    https://doi.org/10.1021/acsami.3c04805
    Published June 20, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    Mn-based cation-disordered rocksalt oxides (Mn-DRX) are emerging as promising cathode materials for next-generation Li-ion batteries due to their high specific capacities and cobalt- and nickel-free characteristic. However, to reach the usable capacity, solid-state synthesized Mn-DRX materials require activation via postsynthetic ball milling, typically incorporating more than 20 wt % conductive carbon that adversely reduces the electrode-level gravimetric capacity. To address this issue, we first deposit amorphous carbon on the surface of the Li1.2Mn0.4Ti0.4O2 (LMTO) particles to increase the electrical conductivity by 5 orders of magnitude. Although the cathode material gravimetric first charge capacity reaches 180 mAh/g, its highly irreversible behavior leads to a first discharge capacity of 70 mAh/g. Subsequently, to ensure a good electrical percolation network, the LMTO material is ball-milled with a multiwall carbon nanotube (CNT) to obtain a 78.7 wt % LMTO active material loading in the cathode electrode (LMTO-CNT). As a result, a 210 mAh/g cathode electrode gravimetric first charge and 165 mAh/g first discharge capacity values are obtained, compared to the respective capacity values of 222 and 155 mAh/g for the LMTO material ball-milled with 20 wt % SuperP C65 electrode (LMTO-SP). After 50 cycles, LMTO-CNT delivers a 121 mAh/g electrode gravimetric discharge capacity, largely outperforming the value of 44 mAh/g of LMTO-SP. Our study demonstrates that while ball milling is necessary to achieve a significant amount of capacity of LMTO, a careful selection of additives, such as CNT, effectively reduces the required carbon quantity to achieve a higher electrode gravimetric discharge capacity.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.3c04805.

    • Enlarged format of XRD plots of various LMTO materials; Mn 2p and Ti 2p XPS spectra of various LMTO materials; HADDF images and EELS spectra of LMTO, LMTO-Ar, and LMTO-ArH2 materials; Raman spectra of LMTO and LMTO-CNT materials; and EIS spectra of the LMTO-CNT cathode at different cycled states (PDF)

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    This article is cited by 5 publications.

    1. Yuncheng Zhou, Yuxing Xu, Jiechen Song, Qiangqiang Tan. Preparation and Performance Investigation of Carbon-Coated Li1.2Mn0.2Ti0.6O2/C Cathode Materials. ACS Applied Materials & Interfaces 2024, 16 (39) , 52539-52549. https://doi.org/10.1021/acsami.4c12757
    2. Krishna Prasad Koirala, Lin Jiang, Shripad Patil, Paolo Longo, Zhao Liu, Bert Freitag, Juri Barthel, Ethan C. Self, Yingge Du, Lee Pullan, Ted Tessner, Leslie J. Allen, Wu Xu, Wei Tong, Jagjit Nanda, Chongmin Wang. Direct Mapping of Fluorine in Cation Disordered Rocksalt Cathodes. ACS Energy Letters 2024, 9 (1) , 10-16. https://doi.org/10.1021/acsenergylett.3c02154
    3. Venkata Sai Avvaru, Mateusz Zuba, Beth L. Armstrong, Shilong Wang, Dong-Min Kim, Isik Su Buyuker, Carrie Siu, Brett A Helms, Ozgenur Kahvecioglu, Haegyeom Kim. Aqueous solution-based synthesis approach for carbon-disordered rocksalt composite cathode development and its limitations. Electrochimica Acta 2025, 509 , 145302. https://doi.org/10.1016/j.electacta.2024.145302
    4. Minyi Su, Yu Yan, Yining Sun, Haiying Xie, Yamin Cheng, Jian Xiong, Guodong Jiang. Dual-functional urea induced interface reaction enables the improved cycling stability of cation-disordered Li1.2Ti0.4Mn0.4O2 cathode. Journal of Solid State Electrochemistry 2024, 28 (8) , 2741-2752. https://doi.org/10.1007/s10008-024-05831-8
    5. Shengxing Lu, Jiuxiang Zhang, Mengting Deng, Kexin Rao, Yian Wang, Keyi Sun, Wenbin Fei, Xiaoping Zhang, Mingye Xiao, Ling Wu, Yulei Sui. Suppressing capacity fading and voltage attenuation by constructing organic interlayer in Li1.2Ti0.4Mn0.4O2 cation-disordered cathode. Applied Surface Science 2024, 665 , 160350. https://doi.org/10.1016/j.apsusc.2024.160350
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 26, 31711–31719
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.3c04805
    Published June 20, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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