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Connolly, B. M.; Aragones-Anglada, M.; Gandara-Loe, J.; Danaf, N. A.; Lamb, D. C.; Mehta, J. P.; Vulpe, D.; Wuttke, Stefan; Silvestre-Albero, J.; Moghadam, P. Z.; Wheatley, A. E. H. und Fairen-Jimenez, D. (2019): Tuning porosity in macroscopic monolithic metal-organic frameworks for exceptional natural gas storage. In: Nature Communications, Bd. 10, 2345 [PDF, 3MB]

Abstract

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 airstable, conformed MOFs for commercial gas storage.

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