Tuning porosity in macroscopic monolithic metal-organic frameworks for exceptional natural gas storage.

BM Connolly, M Aragones-Anglada, J Gandara-Loe, NA Danaf, DC Lamb, JP Mehta, D Vulpe, S Wuttke, J Silvestre-Albero, PZ Moghadam, AEH Wheatley, D Fairen-Jimenez

OAI: oai:www.repository.cam.ac.uk:1810/291790 • DOI: 10.17863/CAM.38950

Widespread access to greener energy is required in order to mitigate the effects of climate change. A significant barrier to cleaner natural gas usage lies in the safety/efficiency limitations of storage technology. Despite highly porous metal-organic frameworks (MOFs) demonstrating record-breaking gas-storage capacities, their conventionally powdered morphology renders them non-viable. Traditional powder shaping utilising high pressure or chemical binders collapses porosity or creates low-density structures with reduced volumetric adsorption capacity. Here, we report the engineering of one of the most stable MOFs, Zr-UiO-66, without applying pressure or binders. The process yields centimetre-sized monoliths, displaying high microporosity and bulk density. We report the inclusion of variable, narrow mesopore volumes to the monoliths' macrostructure and use this to optimise the pore-size distribution for gas uptake. The optimised mixed meso/microporous monoliths demonstrate Type II adsorption isotherms to achieve benchmark volumetric working capacities for methane and carbon dioxide. This represents a critical advance in the design of air-stable, conformed MOFs for commercial gas storage.

0904 Chemical Engineering 0306 Physical Chemistry (incl. Structural)