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Catalysts combined with nanoconfinement can improve the sluggish desorption kinetics and poor reversibility of LiBH 4 . However, at high LiBH 4 loading, their hydrogen storage performance is significantly reduced. Herein, a porous carbon-sphere scaffold decorated with Ni nanoparticles (NPs) was synthesised by calcining a Ni metal-organic framework precursor, followed by partial etching of the Ni NPs to fabricate an optimised scaffold with a high surface area and large porosity that accommodates high LiBH 4 loading (up to 60 wt.%) and exhibits remarkable catalyst/nanoconfinement synergy. Owing to the catalytic effect of Ni 2 B (formed in situ during dehydrogenation) and the reduced hydrogen diffusion distances, the 60 wt.% LiBH 4 confined system exhibited enhanced dehydrogenation kinetics with > 87% of the total hydrogen storage capacity released within 30 min at 375 °C. The apparent activation energies were significantly reduced to 110.5 and 98.3 kJ/mol, compared to that of pure LiBH 4 (149.6 kJ/mol). Moreover, partial reversibility was achieved under moderate conditions (75 bar H 2 , 300 °C) with rapid dehydrogenation during cycling.

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