Densified HKUST-1 Monoliths as a Route to High Volumetric and Gravimetric Hydrogen Storage Capacity

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

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.

Citation

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., Silvestre-Albero, J., …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

• Journal Article Type: Article
• Acceptance Date: Jul 8, 2022
• Online Publication Date: Jul 25, 2022
• Publication Date: Aug 3, 2022
• Deposit Date: Jul 29, 2022
• Publicly Available Date: Aug 1, 2022
• Journal: Journal of the American Chemical Society
• Print ISSN: 0002-7863
• Electronic ISSN: 1520-5126
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• Volume: 144
• Issue: 30
• Pages: 13729-13739
• DOI: https://doi.org/10.1021/jacs.2c04608
• Keywords: Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis
• Public URL: https://nottingham-repository.worktribe.com/output/9409595
• Publisher URL: https://pubs.acs.org/doi/10.1021/jacs.2c04608