Novel Frameworks for Hydrogen Storage

As the world moves to a carbon-free economy, hydrogen poses as a viable alternative to carbon-based energy sources but its current storage methods typically consume a high proportion of the hydrogen’s energy. Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) are tailorable, structured porous materials which can store hydrogen through adsorption.

This thesis discusses the use of high-valency frameworks for H2 storage, presents the first systematic evaluation of the suitability for H2 storage in high-valency 3D COFs, and finally, the design and synthesis of two novel high-valency frameworks, cee-VUF-1 and kew-VUF- 1. cee-VUF-1 has a simulated deliverable H2 capacity of 34.2 g L-1 and 3.3 wt. %, kew-VUF- 1 has a simulated deliverable H2 capacity of 57.6 g L-1 and 11.2 wt. %, surpassing the DoE’s final H2 storage targets of 6.5 wt. %, 50 g L−1. These results showcase how frameworks for gas storage can be guided by high-valency framework design and the use of computational pre-assessment.