Densified HKUST-1 monoliths as a route to high volumetric and gravimetric hydrogen storage capacity

David Gerard Madden; Daniel O'Nolan; Nakul Rampal; Robin Babu; Ceren Çamur; Ali N. Al Shakhs; Shi Yuan Zhang; Graham A. Rance; Javier Perez; Nicola Pietro Maria Casati; Carlos Cuadrado-Collados; Denis O'Sullivan; Nicholas P. Rice; Thomas Gennett; Philip Parilla; Sarah Shulda; Katherine E. Hurst; Vitalie Stavila; Mark D. Allendorf; Joaquin Silvestre-Albero; Alexander C. Forse; Neil R. Champness; Karena W. Chapman; David Fairen-Jimenez

doi:10.1021/jacs.2c04608

Densified HKUST-1 monoliths as a route to high volumetric and gravimetric hydrogen storage capacity

David Gerard Madden^*, Daniel O'Nolan, Nakul Rampal, Robin Babu, Ceren Çamur, Ali N. Al Shakhs, Shi Yuan Zhang, Graham A. Rance, Javier Perez, Nicola Pietro Maria Casati, Carlos Cuadrado-Collados, Denis O'Sullivan, Nicholas P. Rice, Thomas Gennett, Philip Parilla, Sarah Shulda, Katherine E. Hurst, Vitalie Stavila, Mark D. Allendorf, Joaquin Silvestre-AlberoAlexander C. Forse, Neil R. Champness, Karena W. Chapman, David Fairen-Jimenez

^*Corresponding author for this work

Chemistry

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Abstract

We are currently witnessing the dawn of hydrogen (H2) economy, where H2 will soon become a primary fuel for heating, transportation, and long-distance and long-term energy storage. Among diverse possibilities, H2 can be stored as a pressurized gas, a cryogenic liquid, or a solid fuel via adsorption onto porous materials. Metal-organic frameworks (MOFs) have emerged as adsorbent materials with the highest theoretical H2 storage densities on both a volumetric and gravimetric basis. However, a critical bottleneck for the use of H2 as a transportation fuel has been the lack of densification methods capable of shaping MOFs into practical formulations while maintaining their adsorptive performance. Here, we report a high-throughput screening and deep analysis of a database of MOFs to find optimal materials, followed by the synthesis, characterization, and performance evaluation of an optimal monolithic MOF (monoMOF) for H2 storage. After densification, this monoMOF stores 46 g L-1 H2 at 50 bar and 77 K and delivers 41 and 42 g L-1 H2 at operating pressures of 25 and 50 bar, respectively, when deployed in a combined temperature-pressure (25-50 bar/77 K → 5 bar/160 K) swing gas delivery system. This performance represents up to an 80% reduction in the operating pressure requirements for delivering H2 gas when compared with benchmark materials and an 83% reduction compared to compressed H2 gas. Our findings represent a substantial step forward in the application of high-density materials for volumetric H2 storage applications.

Original language	English
Pages (from-to)	13729-13739
Number of pages	11
Journal	Journal of the American Chemical Society
Volume	144
Issue number	30
DOIs	https://doi.org/10.1021/jacs.2c04608
Publication status	Published - 25 Jul 2022

Bibliographical note

Funding Information:
D.F.-J. thanks the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (NanoMOFdeli), ERC-2016-COG 726380, Innovate UK (104384), and EPSRC IAA (IAA/RG85685). D.G.M. acknowledges the SFI-IRC Pathways award (21/PATH-S/9648) from Science Foundation Ireland and the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant Agreement No. 801165 (Project ID: MF20210297). J.S.A. would like to acknowledge the financial support from MINECO (PID2019-108453GB-C21 and PCI2020-111968). N.R.C. thanks the Engineering and Physical Sciences Research Council, United Kingdom (EP/S002995/1), for support. This work was also supported by a UKRI Future Leaders Fellowship to A.C.F. (MR/T043024/1). M.D.A. and V.S. gratefully acknowledge research support from the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office through the Hydrogen Storage Materials Advanced Research Consortium (HyMARC). Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. The authors acknowledge SOLEIL for the provision of the synchrotron radiation facility and the SWING beamline for access to the instrumentation (Project no. 20200126). N.R. acknowledges the support of the Cambridge International Scholarship and the Trinity Henry Barlow Scholarship (Honorary). We also thank Prof. Omar Farha (Northwestern University) and Prof. Donald Siegel (University of Michigan) for providing .cif files for NU-1500-Al and UMCM-9, respectively.

Publisher Copyright:
© 2022 American Chemical Society.

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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Cite this

Madden, D. G., O'Nolan, D., Rampal, N., Babu, R., Çamur, C., Al Shakhs, A. N., Zhang, S. Y., Rance, G. A., Perez, J., Maria Casati, N. P., Cuadrado-Collados, C., O'Sullivan, D., Rice, N. P., Gennett, T., Parilla, P., Shulda, S., Hurst, K. E., Stavila, V., Allendorf, M. D., ... Fairen-Jimenez, D. (2022). Densified HKUST-1 monoliths as a route to high volumetric and gravimetric hydrogen storage capacity. Journal of the American Chemical Society, 144(30), 13729-13739. https://doi.org/10.1021/jacs.2c04608

@article{772ba52553484b70be30c86c8f530aa7,

title = "Densified HKUST-1 monoliths as a route to high volumetric and gravimetric hydrogen storage capacity",

abstract = "We are currently witnessing the dawn of hydrogen (H2) economy, where H2 will soon become a primary fuel for heating, transportation, and long-distance and long-term energy storage. Among diverse possibilities, H2 can be stored as a pressurized gas, a cryogenic liquid, or a solid fuel via adsorption onto porous materials. Metal-organic frameworks (MOFs) have emerged as adsorbent materials with the highest theoretical H2 storage densities on both a volumetric and gravimetric basis. However, a critical bottleneck for the use of H2 as a transportation fuel has been the lack of densification methods capable of shaping MOFs into practical formulations while maintaining their adsorptive performance. Here, we report a high-throughput screening and deep analysis of a database of MOFs to find optimal materials, followed by the synthesis, characterization, and performance evaluation of an optimal monolithic MOF (monoMOF) for H2 storage. After densification, this monoMOF stores 46 g L-1 H2 at 50 bar and 77 K and delivers 41 and 42 g L-1 H2 at operating pressures of 25 and 50 bar, respectively, when deployed in a combined temperature-pressure (25-50 bar/77 K → 5 bar/160 K) swing gas delivery system. This performance represents up to an 80% reduction in the operating pressure requirements for delivering H2 gas when compared with benchmark materials and an 83% reduction compared to compressed H2 gas. Our findings represent a substantial step forward in the application of high-density materials for volumetric H2 storage applications.",

author = "Madden, {David Gerard} and Daniel O'Nolan and Nakul Rampal and Robin Babu and Ceren {\c C}amur and {Al Shakhs}, {Ali N.} and Zhang, {Shi Yuan} and Rance, {Graham A.} and Javier Perez and {Maria Casati}, {Nicola Pietro} and Carlos Cuadrado-Collados and Denis O'Sullivan and Rice, {Nicholas P.} and Thomas Gennett and Philip Parilla and Sarah Shulda and Hurst, {Katherine E.} and Vitalie Stavila and Allendorf, {Mark D.} and Joaquin Silvestre-Albero and Forse, {Alexander C.} and Champness, {Neil R.} and Chapman, {Karena W.} and David Fairen-Jimenez",

note = "Funding Information: D.F.-J. thanks the European Research Council (ERC) under the European Union{\textquoteright}s Horizon 2020 research and innovation programme (NanoMOFdeli), ERC-2016-COG 726380, Innovate UK (104384), and EPSRC IAA (IAA/RG85685). D.G.M. acknowledges the SFI-IRC Pathways award (21/PATH-S/9648) from Science Foundation Ireland and the European Union{\textquoteright}s Horizon 2020 research and innovation programme under the Marie Sk{\l}odowska-Curie grant Agreement No. 801165 (Project ID: MF20210297). J.S.A. would like to acknowledge the financial support from MINECO (PID2019-108453GB-C21 and PCI2020-111968). N.R.C. thanks the Engineering and Physical Sciences Research Council, United Kingdom (EP/S002995/1), for support. This work was also supported by a UKRI Future Leaders Fellowship to A.C.F. (MR/T043024/1). M.D.A. and V.S. gratefully acknowledge research support from the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office through the Hydrogen Storage Materials Advanced Research Consortium (HyMARC). Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy{\textquoteright}s National Nuclear Security Administration under contract DE-NA0003525. The authors acknowledge SOLEIL for the provision of the synchrotron radiation facility and the SWING beamline for access to the instrumentation (Project no. 20200126). N.R. acknowledges the support of the Cambridge International Scholarship and the Trinity Henry Barlow Scholarship (Honorary). We also thank Prof. Omar Farha (Northwestern University) and Prof. Donald Siegel (University of Michigan) for providing .cif files for NU-1500-Al and UMCM-9, respectively. Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = jul,

day = "25",

doi = "10.1021/jacs.2c04608",

language = "English",

volume = "144",

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journal = "Journal of the American Chemical Society",

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Madden, DG, O'Nolan, D, Rampal, N, Babu, R, Çamur, C, Al Shakhs, AN, Zhang, SY, Rance, GA, Perez, J, Maria Casati, NP, Cuadrado-Collados, C, O'Sullivan, D, Rice, NP, Gennett, T, Parilla, P, Shulda, S, Hurst, KE, Stavila, V, Allendorf, MD, Silvestre-Albero, J, Forse, AC, Champness, NR, Chapman, KW & Fairen-Jimenez, D 2022, 'Densified HKUST-1 monoliths as a route to high volumetric and gravimetric hydrogen storage capacity', Journal of the American Chemical Society, vol. 144, no. 30, pp. 13729-13739. https://doi.org/10.1021/jacs.2c04608

TY - JOUR

T1 - Densified HKUST-1 monoliths as a route to high volumetric and gravimetric hydrogen storage capacity

AU - Madden, David Gerard

AU - O'Nolan, Daniel

AU - Rampal, Nakul

AU - Babu, Robin

AU - Çamur, Ceren

AU - Al Shakhs, Ali N.

AU - Zhang, Shi Yuan

AU - Rance, Graham A.

AU - Perez, Javier

AU - Maria Casati, Nicola Pietro

AU - Cuadrado-Collados, Carlos

AU - O'Sullivan, Denis

AU - Rice, Nicholas P.

AU - Gennett, Thomas

AU - Parilla, Philip

AU - Shulda, Sarah

AU - Hurst, Katherine E.

AU - Stavila, Vitalie

AU - Allendorf, Mark D.

AU - Silvestre-Albero, Joaquin

AU - Forse, Alexander C.

AU - Champness, Neil R.

AU - Chapman, Karena W.

AU - Fairen-Jimenez, David

N1 - Funding Information: D.F.-J. thanks the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (NanoMOFdeli), ERC-2016-COG 726380, Innovate UK (104384), and EPSRC IAA (IAA/RG85685). D.G.M. acknowledges the SFI-IRC Pathways award (21/PATH-S/9648) from Science Foundation Ireland and the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant Agreement No. 801165 (Project ID: MF20210297). J.S.A. would like to acknowledge the financial support from MINECO (PID2019-108453GB-C21 and PCI2020-111968). N.R.C. thanks the Engineering and Physical Sciences Research Council, United Kingdom (EP/S002995/1), for support. This work was also supported by a UKRI Future Leaders Fellowship to A.C.F. (MR/T043024/1). M.D.A. and V.S. gratefully acknowledge research support from the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office through the Hydrogen Storage Materials Advanced Research Consortium (HyMARC). Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. The authors acknowledge SOLEIL for the provision of the synchrotron radiation facility and the SWING beamline for access to the instrumentation (Project no. 20200126). N.R. acknowledges the support of the Cambridge International Scholarship and the Trinity Henry Barlow Scholarship (Honorary). We also thank Prof. Omar Farha (Northwestern University) and Prof. Donald Siegel (University of Michigan) for providing .cif files for NU-1500-Al and UMCM-9, respectively. Publisher Copyright: © 2022 American Chemical Society.

PY - 2022/7/25

Y1 - 2022/7/25

N2 - We are currently witnessing the dawn of hydrogen (H2) economy, where H2 will soon become a primary fuel for heating, transportation, and long-distance and long-term energy storage. Among diverse possibilities, H2 can be stored as a pressurized gas, a cryogenic liquid, or a solid fuel via adsorption onto porous materials. Metal-organic frameworks (MOFs) have emerged as adsorbent materials with the highest theoretical H2 storage densities on both a volumetric and gravimetric basis. However, a critical bottleneck for the use of H2 as a transportation fuel has been the lack of densification methods capable of shaping MOFs into practical formulations while maintaining their adsorptive performance. Here, we report a high-throughput screening and deep analysis of a database of MOFs to find optimal materials, followed by the synthesis, characterization, and performance evaluation of an optimal monolithic MOF (monoMOF) for H2 storage. After densification, this monoMOF stores 46 g L-1 H2 at 50 bar and 77 K and delivers 41 and 42 g L-1 H2 at operating pressures of 25 and 50 bar, respectively, when deployed in a combined temperature-pressure (25-50 bar/77 K → 5 bar/160 K) swing gas delivery system. This performance represents up to an 80% reduction in the operating pressure requirements for delivering H2 gas when compared with benchmark materials and an 83% reduction compared to compressed H2 gas. Our findings represent a substantial step forward in the application of high-density materials for volumetric H2 storage applications.

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Densified HKUST-1 monoliths as a route to high volumetric and gravimetric hydrogen storage capacity

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