Small-pore hydridic frameworks store densely packed hydrogen

Hyunchul Oh; Nikolay Tumanov; Voraksmy Ban; Xiao Li; Bo Richter; Matthew R. Hudson; Craig M. Brown; Gail N. Iles; Dirk Wallacher; Scott W. Jorgensen; Luke Daemen; Rafael Balderas-Xicohténcatl; Yongqiang Cheng; Anibal J. Ramirez-Cuesta; Michael Heere; Sergio Posada-Pérez; Geoffroy Hautier; Michael Hirscher; Torben R. Jensen; Yaroslav Filinchuk

doi:10.1038/s41557-024-01443-x

Small-pore hydridic frameworks store densely packed hydrogen

Hyunchul Oh, Nikolay Tumanov, Voraksmy Ban, Xiao Li, Bo Richter, Matthew R. Hudson, Craig M. Brown, Gail N. Iles, Dirk Wallacher, Scott W. Jorgensen, Luke Daemen, Rafael Balderas-Xicohténcatl, Yongqiang Cheng, Anibal J. Ramirez-Cuesta, Michael Heere, Sergio Posada-Pérez, Geoffroy Hautier, Michael Hirscher, Torben R. Jensen, Yaroslav Filinchuk

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

Nanoporous materials have attracted great attention for gas storage, but achieving high volumetric storage capacity remains a challenge. Here, by using neutron powder diffraction, volumetric gas adsorption, inelastic neutron scattering and first-principles calculations, we investigate a magnesium borohydride framework that has small pores and a partially negatively charged non-flat interior for hydrogen and nitrogen uptake. Hydrogen and nitrogen occupy distinctly different adsorption sites in the pores, with very different limiting capacities of 2.33 H₂ and 0.66 N₂ per Mg(BH₄)₂. Molecular hydrogen is packed extremely densely, with about twice the density of liquid hydrogen (144 g H₂ per litre of pore volume). We found a penta-dihydrogen cluster where H₂ molecules in one position have rotational freedom, whereas H₂ molecules in another position have a well-defined orientation and a directional interaction with the framework. This study reveals that densely packed hydrogen can be stabilized in small-pore materials at ambient pressures. (Figure presented.)

Original language	English
Pages (from-to)	809-816
Number of pages	8
Journal	Nature Chemistry
Volume	16
Issue number	5
DOIs	https://doi.org/10.1038/s41557-024-01443-x
State	Published - May 2024
Externally published	Yes

Funding

H.O. is grateful for partial funding by the National Research Foundation of Korea (NRF) (grant 2022R1A2C3005978). Partial funding by the German Research Foundation (DFG) within the priority programme SSP 1362 is gratefully acknowledged. We thank the F.R.S.-FNRS (Belgium), the Fonds Sp\u00E9ciaux de Recherche (UCL), F\u00E9d\u00E9ration Wallonie-Bruxelles (ARC 18/23-093 MicroBat) and General Motors Global R&D for financial support. We acknowledge the support of NIST, the US Department of Commerce and Helmholtz-Zentrum Berlin in providing the neutron research facilities used in this work. Neutron beam time at Helmholtz-Zentrum Berlin was awarded via funding proposal CHE-01-3161. The work was supported by The Danish Research Council for Nature and Universe (Danscatt) and by The Independent Research Fund Denmark for Technology and Production (9041-00226B). We are grateful to the Carlsberg Foundation and China Scholarship Council for the fellowship of X. Li (CSC201706370133). The neutron scattering experiment was performed at ORNL\u2019s Spallation Neutron Source, supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy, under contract no. DE-AC0500OR22725 with UT Battelle. R.B.-X. gratefully acknowledges research support from the Hydrogen Materials\u2014Advanced Research Consortium (HyMARC), established as part of the Energy Materials Network under the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office, under contract no. DE-AC05-00OR22725. S.P.-P. acknowledges a Marie Curie fellowship (H2020-MSCA-IF-2020-101020330). Computational time at the MARENOSTRUM supercomputer was provided by the Barcelona Supercomputing Centre through a grant from Red Espa\u00F1ola de Supercomputaci\u00F3n (QHS-2022-3-0003).

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Oh, H., Tumanov, N., Ban, V., Li, X., Richter, B., Hudson, M. R., Brown, C. M., Iles, G. N., Wallacher, D., Jorgensen, S. W., Daemen, L., Balderas-Xicohténcatl, R., Cheng, Y., Ramirez-Cuesta, A. J., Heere, M., Posada-Pérez, S., Hautier, G., Hirscher, M., Jensen, T. R., & Filinchuk, Y. (2024). Small-pore hydridic frameworks store densely packed hydrogen. Nature Chemistry, 16(5), 809-816. https://doi.org/10.1038/s41557-024-01443-x

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abstract = "Nanoporous materials have attracted great attention for gas storage, but achieving high volumetric storage capacity remains a challenge. Here, by using neutron powder diffraction, volumetric gas adsorption, inelastic neutron scattering and first-principles calculations, we investigate a magnesium borohydride framework that has small pores and a partially negatively charged non-flat interior for hydrogen and nitrogen uptake. Hydrogen and nitrogen occupy distinctly different adsorption sites in the pores, with very different limiting capacities of 2.33 H2 and 0.66 N2 per Mg(BH4)2. Molecular hydrogen is packed extremely densely, with about twice the density of liquid hydrogen (144 g H2 per litre of pore volume). We found a penta-dihydrogen cluster where H2 molecules in one position have rotational freedom, whereas H2 molecules in another position have a well-defined orientation and a directional interaction with the framework. This study reveals that densely packed hydrogen can be stabilized in small-pore materials at ambient pressures. (Figure presented.)",

author = "Hyunchul Oh and Nikolay Tumanov and Voraksmy Ban and Xiao Li and Bo Richter and Hudson, {Matthew R.} and Brown, {Craig M.} and Iles, {Gail N.} and Dirk Wallacher and Jorgensen, {Scott W.} and Luke Daemen and Rafael Balderas-Xicoht{\'e}ncatl and Yongqiang Cheng and Ramirez-Cuesta, {Anibal J.} and Michael Heere and Sergio Posada-P{\'e}rez and Geoffroy Hautier and Michael Hirscher and Jensen, {Torben R.} and Yaroslav Filinchuk",

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Oh, H, Tumanov, N, Ban, V, Li, X, Richter, B, Hudson, MR, Brown, CM, Iles, GN, Wallacher, D, Jorgensen, SW, Daemen, L, Balderas-Xicohténcatl, R, Cheng, Y , Ramirez-Cuesta, AJ, Heere, M, Posada-Pérez, S, Hautier, G, Hirscher, M, Jensen, TR & Filinchuk, Y 2024, 'Small-pore hydridic frameworks store densely packed hydrogen', Nature Chemistry, vol. 16, no. 5, pp. 809-816. https://doi.org/10.1038/s41557-024-01443-x

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AU - Tumanov, Nikolay

AU - Ban, Voraksmy

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AU - Brown, Craig M.

AU - Iles, Gail N.

AU - Wallacher, Dirk

AU - Jorgensen, Scott W.

AU - Daemen, Luke

AU - Balderas-Xicohténcatl, Rafael

AU - Cheng, Yongqiang

AU - Ramirez-Cuesta, Anibal J.

AU - Heere, Michael

AU - Posada-Pérez, Sergio

AU - Hautier, Geoffroy

AU - Hirscher, Michael

AU - Jensen, Torben R.

AU - Filinchuk, Yaroslav

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N2 - Nanoporous materials have attracted great attention for gas storage, but achieving high volumetric storage capacity remains a challenge. Here, by using neutron powder diffraction, volumetric gas adsorption, inelastic neutron scattering and first-principles calculations, we investigate a magnesium borohydride framework that has small pores and a partially negatively charged non-flat interior for hydrogen and nitrogen uptake. Hydrogen and nitrogen occupy distinctly different adsorption sites in the pores, with very different limiting capacities of 2.33 H2 and 0.66 N2 per Mg(BH4)2. Molecular hydrogen is packed extremely densely, with about twice the density of liquid hydrogen (144 g H2 per litre of pore volume). We found a penta-dihydrogen cluster where H2 molecules in one position have rotational freedom, whereas H2 molecules in another position have a well-defined orientation and a directional interaction with the framework. This study reveals that densely packed hydrogen can be stabilized in small-pore materials at ambient pressures. (Figure presented.)

AB - Nanoporous materials have attracted great attention for gas storage, but achieving high volumetric storage capacity remains a challenge. Here, by using neutron powder diffraction, volumetric gas adsorption, inelastic neutron scattering and first-principles calculations, we investigate a magnesium borohydride framework that has small pores and a partially negatively charged non-flat interior for hydrogen and nitrogen uptake. Hydrogen and nitrogen occupy distinctly different adsorption sites in the pores, with very different limiting capacities of 2.33 H2 and 0.66 N2 per Mg(BH4)2. Molecular hydrogen is packed extremely densely, with about twice the density of liquid hydrogen (144 g H2 per litre of pore volume). We found a penta-dihydrogen cluster where H2 molecules in one position have rotational freedom, whereas H2 molecules in another position have a well-defined orientation and a directional interaction with the framework. This study reveals that densely packed hydrogen can be stabilized in small-pore materials at ambient pressures. (Figure presented.)

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ER -

Small-pore hydridic frameworks store densely packed hydrogen

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