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.
1.Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England 2.Univ Cambridge, Dept Chem Engn & Biotechnol, AAM Lab, Philippa Fawcett Dr, Cambridge CB3 0AS, England 3.Univ Alicante, Inst Univ Mat, Dept Quim Inorgan, Lab Mat Avanzados, Ctra San Vicente Alicante S-N, E-03690 San Vicente Del Raspeig, Spain 4.Ludwig Maximilians Univ Munchen, Munchen LMU, Dept Chem,Ctr Integrated Prot Sci Munich, Ctr NanoSci CeNS,Nanosyst Initiat Munich, Butenandtstr 11, D-81377 Munich, Germany 5.Univ Lincoln, Sch Chem, Coll Sci, Lincoln LN6 7TS, England 6.Univ Sheffield, Dept Chem & Biol Engn, Mappin St, Sheffield S1 3JD, S Yorkshire, England
Recommended Citation:
Connolly, B. M.,Aragones-Anglada, M.,Gandara-Loe, J.,et al. Tuning porosity in macroscopic monolithic metal-organic frameworks for exceptional natural gas storage[J]. NATURE COMMUNICATIONS,2019-01-01,10