Bambalaza, S.ELangmi, H.WMokaya, R2021-05-202021-05-202021Bambalaza, S.E. et al. (2021). Co-pelletization of a zirconium-based metal-organic framework (UiO-66) with polymer nanofibers for improved useable capacity in hydrogen storage. International Journal of Hydrogen Energy, 46(12), 8607-86200360-319910.1016/j.ijhydene.2020.12.049http://hdl.handle.net/10566/6170We report on a concept of co-pelletization using mechanically robust hydroxylated UiO-66 to develop a metal-organic framework (MOF) monolith that contains 5 wt% electrospun polymer nanofibers, and consists of an architecture with alternating layers of MOF and nanofiber mats. The polymers of choice were the microporous Polymer of Intrinsic Microporosity (PIM-1) and non-porous polyacrylonitrile (PAN). Co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths retain no less than 85% of the porosity obtained in pristine powder and pelletized UiO-66. The composition of the pore size distribution in co-pelletized UiO-66/PIM-1 and UiO-66/PAN monoliths is significantly different to that of pristine UiO-66 forms, with pristine UiO-66 forms showing 90% of the pore apertures in the micropore region and both UiO-66/nanofiber monoliths showing a composite micro-mesoporous pore size distribution. The co-pelletized UiO-66/nanofiber monoliths obtained improved useable H2 capacities in comparison to pristine UiO-66 forms, under isothermal pressure swing conditions. The UiO-66/PIM-1 monolith constitutes the highest gravimetric (and volumetric) useable capacities at 2.3 wt% (32 g L−1) in comparison to 1.8 wt% (12 g L−1) and 1.9 wt% (29 g L−1) obtainable in pristine UiO-66 powder and UiO-66 pellet, respectively.enCo-pelletizationHierarchical porosityHydrogen useable capacityMetal-organicArticle