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

[Image: see text] We are currently witnessing the dawn of hydrogen (H(2)) economy, where H(2) will soon become a primary fuel for heating, transportation, and long-distance and long-term energy storage. Among diverse possibilities, H(2) 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 H(2) storage densities on both a volumetric and gravimetric basis. However, a critical bottleneck for the use of H(2) 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 ((mono)MOF) for H(2) storage. After densification, this (mono)MOF stores 46 g L(–1) H(2) at 50 bar and 77 K and delivers 41 and 42 g L(–1) H(2) 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 H(2) gas when compared with benchmark materials and an 83% reduction compared to compressed H(2) gas. Our findings represent a substantial step forward in the application of high-density materials for volumetric H(2) storage applications.