Amorphized Defective Fullerene with a Single-Atom Platinum for Room-Temperature Hydrogen Storage

摘要

The search for hydrogen storage materials allowing the storage of hydrogenin its molecular or atomic form at room temperature to meet the multistagetargets such as the US Department of Energy (DOE) ultimate gravimetric andvolumetric capacities of 6.5 wt and 50 kg m~(-3) is of global importance. Here,it is reported that an amorphized defective fullerene (C_(60-x)) offers a promisingsolution to this challenge. C_(60-x) immobilized with single-atom platinumhas ≈14-fold higher surface area accessible for C-H bonds compared to acrystalline C_(60), and its micro/meso pores give a ≈20-fold larger volume forfast hydrogen transport. Indeed, hydrogen storage via spillover on C_(60)through pressure swing at room temperature is experimentally demonstratedto enable high reversible gravimetric (6.8 wt) and volumetric (64.9 kg m~(-3))capacities, hitherto the highest reversible capacities close to DOE targets atroom temperature. Also, the density functional theory calculations show thata key to efficient hydrogen storage is the preservation of a curved sp~2-typelocal carbon geometry for spillover, which holds H radicals loosely for fasthydrogen migration. Moreover, H-atom diffusion on the intact region of C_(60)is faster than that on the defect region. Furthermore, excellent capacity retentionis achieved over repeated hydrogen adsorption/desorption cycles.