Balancing volumetric and gravimetric capacity for hydrogen in supramolecular crystals

Ruihua Zhang; Hilal Daglar; Chun Tang; Penghao Li; Liang Feng; Han Han; Guangcheng Wu; Benjie N. Limketkai; Yong Wu; Shuliang Yang; Aspen X.Y. Chen; Charlotte L. Stern; Christos D. Malliakas; Randall Q. Snurr; J. Fraser Stoddart

doi:10.1038/s41557-024-01622-w

Balancing volumetric and gravimetric capacity for hydrogen in supramolecular crystals

Ruihua Zhang, Hilal Daglar, Chun Tang^*, Penghao Li, Liang Feng, Han Han, Guangcheng Wu, Benjie N. Limketkai, Yong Wu, Shuliang Yang, Aspen X.Y. Chen, Charlotte L. Stern, Christos D. Malliakas, Randall Q. Snurr^*, J. Fraser Stoddart^*

^*Corresponding author for this work

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

10 Scopus citations

Abstract

The storage of hydrogen is key to its applications. Developing adsorbent materials with high volumetric and gravimetric storage capacities, both of which are essential for the efficient use of hydrogen as a fuel, is challenging. Here we report a controlled catenation strategy in hydrogen-bonded organic frameworks (RP-H100 and RP-H101) that depends on multiple hydrogen bonds to guide catenation in a point-contact manner, resulting in high volumetric and gravimetric surface areas, robustness and ideal pore diameters (~1.2–1.9 nm) for hydrogen storage. This approach involves assembling nine imidazole-annulated triptycene hexaacids into a secondary hexagonal superstructure containing three open channels through which seven of the hexagons interpenetrate to form a seven-fold catenated superstructure. RP-H101 exhibits high deliverable volumetric (53.7 g l⁻¹) and gravimetric (9.3 wt%) capacities for hydrogen under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar). This work illustrates the virtues of supramolecular crystals as promising candidates for hydrogen storage. (Figure presented.)

Original language	English (US)
Pages (from-to)	1982-1988
Number of pages	7
Journal	Nature chemistry
Volume	16
Issue number	12
DOIs	https://doi.org/10.1038/s41557-024-01622-w
State	Published - Dec 2024

Funding

We acknowledge D. Kiska (Anton Paar), O. M. Yaghi and Z. Zheng (UC Berkeley), as well as Z. Lin, H. Xie and K. B. Idrees (Northwestern University), for experimental help and discussions. We also acknowledge support in carrying out the high-pressure characterization of RP-H101 by W. Wang, L. Long, Y.-B. Zhang and the Analytical Instrumentation Center (SPST-AIC10112914) at ShanghaiTech University. We thank Northwestern University (NU), the University of Hong Kong and H2MOF, Inc. for their financial support, and acknowledge the Integrated Molecular Structure Education and Research Centre at NU for providing access to equipment for relevant experiments. We acknowledge support from the US Department of Energy\u2019s Office of Energy Efficiency and Renewable Energy under grant no. DE-EE0008816 (R.Q.S.). We also gratefully acknowledge the resources provided by the National Energy Research Scientific Computing Centre (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under contract no. DE-AC02-05CH11231 using NERSC award BES-ERCAP0023154 (R.Q.S.). H.D. is supported by the Scientific and Technological Research Council of Turkey (TUBITAK) 2214-A (decision no. 1059B142200109).

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering

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10.1038/s41557-024-01622-w

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title = "Balancing volumetric and gravimetric capacity for hydrogen in supramolecular crystals",

abstract = "The storage of hydrogen is key to its applications. Developing adsorbent materials with high volumetric and gravimetric storage capacities, both of which are essential for the efficient use of hydrogen as a fuel, is challenging. Here we report a controlled catenation strategy in hydrogen-bonded organic frameworks (RP-H100 and RP-H101) that depends on multiple hydrogen bonds to guide catenation in a point-contact manner, resulting in high volumetric and gravimetric surface areas, robustness and ideal pore diameters (~1.2–1.9 nm) for hydrogen storage. This approach involves assembling nine imidazole-annulated triptycene hexaacids into a secondary hexagonal superstructure containing three open channels through which seven of the hexagons interpenetrate to form a seven-fold catenated superstructure. RP-H101 exhibits high deliverable volumetric (53.7 g l−1) and gravimetric (9.3 wt%) capacities for hydrogen under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar). This work illustrates the virtues of supramolecular crystals as promising candidates for hydrogen storage. (Figure presented.)",

author = "Ruihua Zhang and Hilal Daglar and Chun Tang and Penghao Li and Liang Feng and Han Han and Guangcheng Wu and Limketkai, {Benjie N.} and Yong Wu and Shuliang Yang and Chen, {Aspen X.Y.} and Stern, {Charlotte L.} and Malliakas, {Christos D.} and Snurr, {Randall Q.} and Stoddart, {J. Fraser}",

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AU - Wu, Guangcheng

AU - Limketkai, Benjie N.

AU - Wu, Yong

AU - Yang, Shuliang

AU - Chen, Aspen X.Y.

AU - Stern, Charlotte L.

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N2 - The storage of hydrogen is key to its applications. Developing adsorbent materials with high volumetric and gravimetric storage capacities, both of which are essential for the efficient use of hydrogen as a fuel, is challenging. Here we report a controlled catenation strategy in hydrogen-bonded organic frameworks (RP-H100 and RP-H101) that depends on multiple hydrogen bonds to guide catenation in a point-contact manner, resulting in high volumetric and gravimetric surface areas, robustness and ideal pore diameters (~1.2–1.9 nm) for hydrogen storage. This approach involves assembling nine imidazole-annulated triptycene hexaacids into a secondary hexagonal superstructure containing three open channels through which seven of the hexagons interpenetrate to form a seven-fold catenated superstructure. RP-H101 exhibits high deliverable volumetric (53.7 g l−1) and gravimetric (9.3 wt%) capacities for hydrogen under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar). This work illustrates the virtues of supramolecular crystals as promising candidates for hydrogen storage. (Figure presented.)

AB - The storage of hydrogen is key to its applications. Developing adsorbent materials with high volumetric and gravimetric storage capacities, both of which are essential for the efficient use of hydrogen as a fuel, is challenging. Here we report a controlled catenation strategy in hydrogen-bonded organic frameworks (RP-H100 and RP-H101) that depends on multiple hydrogen bonds to guide catenation in a point-contact manner, resulting in high volumetric and gravimetric surface areas, robustness and ideal pore diameters (~1.2–1.9 nm) for hydrogen storage. This approach involves assembling nine imidazole-annulated triptycene hexaacids into a secondary hexagonal superstructure containing three open channels through which seven of the hexagons interpenetrate to form a seven-fold catenated superstructure. RP-H101 exhibits high deliverable volumetric (53.7 g l−1) and gravimetric (9.3 wt%) capacities for hydrogen under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar). This work illustrates the virtues of supramolecular crystals as promising candidates for hydrogen storage. (Figure presented.)

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Balancing volumetric and gravimetric capacity for hydrogen in supramolecular crystals

Abstract

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