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Title: Hierarchically Controlled Inside-Out Doping of Mg Nanocomposites for Moderate Temperature Hydrogen Storage

Demand for pragmatic alternatives to carbon–intensive fossil fuels is growing more strident. Hydrogen represents an ideal zero–carbon clean energy carrier with high energy density. For hydrogen fuel to compete with alternatives, safe and high capacity storage materials that are readily cycled are imperative. Here, development of such a material, comprised of nickel–doped Mg nanocrystals encapsulated by molecular–sieving reduced graphene oxide (rGO) layers, is reported. While most work on advanced hydrogen storage composites to date endeavor to explore either nanosizing or addition of carbon materials as secondary additives individually, methods to enable both are pioneered: “dual–channel” doping combines the benefits of two different modalities of enhancement. Specifically, both external (rGO strain) and internal (Ni doping) mechanisms are used to efficiently promote both hydriding and dehydriding processes of Mg nanocrystals, simultaneously achieving high hydrogen storage capacity (6.5 wt% in the total composite) and excellent kinetics while maintaining robustness. Furthermore, hydrogen uptake is remarkably accomplished at room temperature and also under 1 bar—as observed during in situ measurements—which is a substantial advance for a reversible metal hydride material. In conclusion, the realization of three complementary functional components in one material breaks new ground in metal hydrides and makes solid–state materials viable candidates formore » hydrogen–fueled applications.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5] ;  [6] ;  [3] ;  [6] ;  [7] ;  [4] ;  [3] ;  [4] ;  [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Korea Advanced Inst. of Science and Technology (KAIST), Daejeon (Republic of Korea). Dept. of Chemical and Biomolecular Engineering
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Materials Science Division
  4. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  7. Korea Advanced Inst. of Science and Technology (KAIST), Daejeon (Republic of Korea). Dept. of Chemical and Biomolecular Engineering
Publication Date:
Report Number(s):
LLNL-JRNL-722239; SAND2018-10164J
Journal ID: ISSN 1616-301X; 861906
Grant/Contract Number:
AC52-07NA27344; AC02‐05CH11231; EE0004946; AC36‐08GO28308; IUSSTF/JCERDC‐SERIIUS/2012; AC04-94AL85000
Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 47; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S); Ministry Of Science And Technology, Dept. of Science and Technology (DST) (India)
Contributing Orgs:
Bay Area Photovoltaic Consortium (BAPVC); Partnership to Advance Clean Energy Research (PACE-R)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 08 HYDROGEN; dual doping; fuel cell electric vehicle (FCEV); hydrogen storage; magnesium
OSTI Identifier:
1461741
Alternate Identifier(s):
OSTI ID: 1402521; OSTI ID: 1474048

Cho, Eun Seon, Ruminski, Anne M., Liu, Yi -Sheng, Shea, Patrick T., Kang, Shin Young, Zaia, Edmond W., Park, Jae Yeol, Chuang, Yi -De, Yuk, Jong Min, Zhou, Xiaowang, Heo, Tae Wook, Guo, Jinghua, Wood, Brandon C., and Urban, Jeffrey J.. Hierarchically Controlled Inside-Out Doping of Mg Nanocomposites for Moderate Temperature Hydrogen Storage. United States: N. p., Web. doi:10.1002/adfm.201704316.
Cho, Eun Seon, Ruminski, Anne M., Liu, Yi -Sheng, Shea, Patrick T., Kang, Shin Young, Zaia, Edmond W., Park, Jae Yeol, Chuang, Yi -De, Yuk, Jong Min, Zhou, Xiaowang, Heo, Tae Wook, Guo, Jinghua, Wood, Brandon C., & Urban, Jeffrey J.. Hierarchically Controlled Inside-Out Doping of Mg Nanocomposites for Moderate Temperature Hydrogen Storage. United States. doi:10.1002/adfm.201704316.
Cho, Eun Seon, Ruminski, Anne M., Liu, Yi -Sheng, Shea, Patrick T., Kang, Shin Young, Zaia, Edmond W., Park, Jae Yeol, Chuang, Yi -De, Yuk, Jong Min, Zhou, Xiaowang, Heo, Tae Wook, Guo, Jinghua, Wood, Brandon C., and Urban, Jeffrey J.. 2017. "Hierarchically Controlled Inside-Out Doping of Mg Nanocomposites for Moderate Temperature Hydrogen Storage". United States. doi:10.1002/adfm.201704316. https://www.osti.gov/servlets/purl/1461741.
@article{osti_1461741,
title = {Hierarchically Controlled Inside-Out Doping of Mg Nanocomposites for Moderate Temperature Hydrogen Storage},
author = {Cho, Eun Seon and Ruminski, Anne M. and Liu, Yi -Sheng and Shea, Patrick T. and Kang, Shin Young and Zaia, Edmond W. and Park, Jae Yeol and Chuang, Yi -De and Yuk, Jong Min and Zhou, Xiaowang and Heo, Tae Wook and Guo, Jinghua and Wood, Brandon C. and Urban, Jeffrey J.},
abstractNote = {Demand for pragmatic alternatives to carbon–intensive fossil fuels is growing more strident. Hydrogen represents an ideal zero–carbon clean energy carrier with high energy density. For hydrogen fuel to compete with alternatives, safe and high capacity storage materials that are readily cycled are imperative. Here, development of such a material, comprised of nickel–doped Mg nanocrystals encapsulated by molecular–sieving reduced graphene oxide (rGO) layers, is reported. While most work on advanced hydrogen storage composites to date endeavor to explore either nanosizing or addition of carbon materials as secondary additives individually, methods to enable both are pioneered: “dual–channel” doping combines the benefits of two different modalities of enhancement. Specifically, both external (rGO strain) and internal (Ni doping) mechanisms are used to efficiently promote both hydriding and dehydriding processes of Mg nanocrystals, simultaneously achieving high hydrogen storage capacity (6.5 wt% in the total composite) and excellent kinetics while maintaining robustness. Furthermore, hydrogen uptake is remarkably accomplished at room temperature and also under 1 bar—as observed during in situ measurements—which is a substantial advance for a reversible metal hydride material. In conclusion, the realization of three complementary functional components in one material breaks new ground in metal hydrides and makes solid–state materials viable candidates for hydrogen–fueled applications.},
doi = {10.1002/adfm.201704316},
journal = {Advanced Functional Materials},
number = 47,
volume = 27,
place = {United States},
year = {2017},
month = {10}
}

Works referenced in this record:

Ultrathin, Molecular-Sieving Graphene Oxide Membranes for Selective Hydrogen Separation
journal, October 2013

Hydrogen dissociation and diffusion on transition metal (=Ti, Zr, V, Fe, Ru, Co, Rh, Ni, Pd, Cu, Ag)-doped Mg(0001) surfaces
journal, February 2009