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Reversing the Irreversible: Thermodynamic Stabilization of LiAlH4 Nanoconfined Within a Nitrogen-Doped Carbon Host

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    Reversing the Irreversible: Thermodynamic Stabilization of LiAlH4 Nanoconfined Within a Nitrogen-Doped Carbon Host
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    • YongJun Cho
      YongJun Cho
      Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
      Department of Chemical and Biomolecular Engineering (BK21+ Program), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
      More by YongJun Cho
    • Sichi Li
      Sichi Li
      Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States
      More by Sichi Li
      Orcidhttps://orcid.org/0000-0002-2565-5906
    • Jonathan L. Snider
      Jonathan L. Snider
      Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
      More by Jonathan L. Snider
    • Maxwell A. T. Marple
      Maxwell A. T. Marple
      Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States
      More by Maxwell A. T. Marple
      Orcidhttps://orcid.org/0000-0001-5251-8301
    • Nicholas A. Strange
      Nicholas A. Strange
      SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States
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      Orcidhttps://orcid.org/0000-0001-5699-7274
    • Joshua D. Sugar
      Joshua D. Sugar
      Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
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    • Farid El Gabaly
      Farid El Gabaly
      Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
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      Orcidhttps://orcid.org/0000-0002-5822-9938
    • Andreas Schneemann
      Andreas Schneemann
      Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
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      Orcidhttps://orcid.org/0000-0001-6801-2735
    • Sungsu Kang
      Sungsu Kang
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea
      More by Sungsu Kang
    • Min-ho Kang
      Min-ho Kang
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea
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    • Hayoung Park
      Hayoung Park
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea
      More by Hayoung Park
    • Jungwon Park
      Jungwon Park
      Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
      School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea
      More by Jungwon Park
      Orcidhttps://orcid.org/0000-0003-2927-4331
    • Liwen F. Wan
      Liwen F. Wan
      Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States
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      Orcidhttps://orcid.org/0000-0002-5391-0804
    • Harris E. Mason
      Harris E. Mason
      Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States
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      Orcidhttps://orcid.org/0000-0002-1840-0550
    • Mark D. Allendorf
      Mark D. Allendorf
      Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
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      Orcidhttps://orcid.org/0000-0001-5645-8246
    • Brandon C. Wood*
      Brandon C. Wood
      Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0002-1450-9719
    • Eun Seon Cho*
      Eun Seon Cho
      Department of Chemical and Biomolecular Engineering (BK21+ Program), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
      *Email: [email protected]
      More by Eun Seon Cho
      Orcidhttps://orcid.org/0000-0001-9428-1269
    • Vitalie Stavila*
      Vitalie Stavila
      Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States
      *Email: [email protected]
      More by Vitalie Stavila
      Orcidhttps://orcid.org/0000-0003-0981-0432
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    ACS Nano

    Cite this: ACS Nano 2021, 15, 6, 10163–10174
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    https://doi.org/10.1021/acsnano.1c02079
    Published May 24, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    A general problem when designing functional nanomaterials for energy storage is the lack of control over the stability and reactivity of metastable phases. Using the high-capacity hydrogen storage candidate LiAlH4 as an exemplar, we demonstrate an alternative approach to the thermodynamic stabilization of metastable metal hydrides by coordination to nitrogen binding sites within the nanopores of N-doped CMK-3 carbon (NCMK-3). The resulting LiAlH4@NCMK-3 material releases H2 at temperatures as low as 126 °C with full decomposition below 240 °C, bypassing the usual Li3AlH6 intermediate observed in bulk. Moreover, >80% of LiAlH4 can be regenerated under 100 MPa H2, a feat previously thought to be impossible. Nitrogen sites are critical to these improvements, as no reversibility is observed with undoped CMK-3. Density functional theory predicts a drastically reduced Al–H bond dissociation energy and supports the observed change in the reaction pathway. The calculations also provide a rationale for the solid-state reversibility, which derives from the combined effects of nanoconfinement, Li adatom formation, and charge redistribution between the metal hydride and the host.

    Copyright © 2021 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/acsnano.1c02079.

    • Figures of pore size distributions, FTIR spectra, PXRD patterns, 7Li MAS NMR spectra, N 1s spectra, schematic illustration of N-functionalities, brightness analysis, HAADF-STEM line profile, EDS signals, EELS profile, hydrogen desorption kinetic curve, high-angle annular dark field EDS map image, relaxed geometries, schematic representation of spontaneous interdiffusion, optimized structures of graphene sheets, ex situ N K-edge soft TEY X-ray absorption spectra, isosurface of charge density difference, and electronic density of states, tables of BET surface areas and total pore volumes, relative amount of various nitrogen functionalities, and NMR parameters, and notes of synthesis and storage methods, identification of the origin of partial LiAlH4 decomposition upon solvent infiltration, detailed description of MAS NMR measurements, and detailed description of theoretical calculations (PDF)

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    This article is cited by 36 publications.

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    Cite this: ACS Nano 2021, 15, 6, 10163–10174
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.1c02079
    Published May 24, 2021
    Copyright © 2021 American Chemical Society
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