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Reversing the Irreversible: Thermodynamic Stabilization of LiAlH4 Nanoconfined Within a Nitrogen-Doped Carbon Host.
Cho, YongJun; Li, Sichi; Snider, Jonathan L; Marple, Maxwell A T; Strange, Nicholas A; Sugar, Joshua D; El Gabaly, Farid; Schneemann, Andreas; Kang, Sungsu; Kang, Min-Ho; Park, Hayoung; Park, Jungwon; Wan, Liwen F; Mason, Harris E; Allendorf, Mark D; Wood, Brandon C; Cho, Eun Seon; Stavila, Vitalie.
Affiliation
  • Cho Y; Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States.
  • Li S; Department of Chemical and Biomolecular Engineering (BK21+ Program), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.
  • Snider JL; Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States.
  • Marple MAT; Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States.
  • Strange NA; Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States.
  • Sugar JD; SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
  • El Gabaly F; Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States.
  • Schneemann A; Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States.
  • Kang S; Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States.
  • Kang MH; Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.
  • Park H; School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea.
  • Park J; Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.
  • Wan LF; School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea.
  • Mason HE; Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.
  • Allendorf MD; School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea.
  • Wood BC; Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.
  • Cho ES; School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, Seoul 08826, Republic of Korea.
  • Stavila V; Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States.
ACS Nano ; 15(6): 10163-10174, 2021 Jun 22.
Article in En | MEDLINE | ID: mdl-34029480
ABSTRACT
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.
Key words

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: ACS Nano Year: 2021 Type: Article Affiliation country: United States

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: ACS Nano Year: 2021 Type: Article Affiliation country: United States