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

Nat Chem. 2024 Dec;16(12):1982-1988. doi: 10.1038/s41557-024-01622-w. Epub 2024 Sep 3.

Authors

Ruihua Zhang^{1

2}, Hilal Daglar³, Chun Tang^{4

5}, Penghao Li², Liang Feng⁶, Han Han^{1

2}, Guangcheng Wu^{1

2}, Benjie N Limketkai⁷, Yong Wu^{1

2}, Shuliang Yang², Aspen X-Y Chen¹, Charlotte L Stern², Christos D Malliakas², Randall Q Snurr⁸, J Fraser Stoddart^{9

10

11

12

13

14

15}

Affiliations

¹ Department of Chemistry, The University of Hong Kong, Hong Kong, China.
² Department of Chemistry, Northwestern University, Evanston, IL, USA.
³ Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL, USA.
⁴ Department of Chemistry, The University of Hong Kong, Hong Kong, China. tangchem@hku.hk.
⁵ Department of Chemistry, Northwestern University, Evanston, IL, USA. tangchem@hku.hk.
⁶ Thomas Lord Department of Mechanical Engineering and Materials Science, Duke University, Durham, NC, USA.
⁷ H2MOF Inc., Irvine, CA, USA.
⁸ Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL, USA. snurr@northwestern.edu.
⁹ Department of Chemistry, The University of Hong Kong, Hong Kong, China. stoddart@hku.hk.
¹⁰ Department of Chemistry, Northwestern University, Evanston, IL, USA. stoddart@hku.hk.
¹¹ H2MOF Inc., Irvine, CA, USA. stoddart@hku.hk.
¹² Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, IL, USA. stoddart@hku.hk.
¹³ Stoddart Institute of Molecular Science, Department of Chemistry, Zhejiang University, Hangzhou, China. stoddart@hku.hk.
¹⁴ ZJU-Hangzhou Global Scientific and Technological Innovation Centre, Hangzhou, China. stoddart@hku.hk.
¹⁵ School of Chemistry, University of New South Wales, Sydney, New South Wales, Australia. stoddart@hku.hk.

PMID: 39227421
DOI: 10.1038/s41557-024-01622-w

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.

Abstract

Grants and funding