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., …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 (ACS)
• 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