• Gandara-Loe, J.
• Danaf, Na
• Wuttke, Stefan
• Fairen-Jimenez, David
• Aragones-Anglada, M.
• Moghadam, Pz
• Lamb, Dc
• Silvestre-Albero, J.
• Wheatley, Aeh
• Connolly, Bm
• Mehta, Jp
• Vulpe, D.

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 air-stable, conformed MOFs for commercial gas storage.

Topics

• porous
• density
• impedance spectroscopy
• pore
• Carbon
• inclusion
• porosity