Electronic metal-support interactions for defect-induced Ru/Co-Sm2O3 mesosphere to achieve efficient NaBH4 hydrolysis activity

Abstract

Crafting resilient catalysts that promote H2 production through the hydrolysis of hydrogen storage materials like sodium borohydride stands paramount for the impending hydrogen economy. In this study, we propose a versatile metal–organic framework (MOF)-assisted approach to systematically explore the impact of electron-metal support interaction (EMSI) of Ru-modified Co-Sm2O3 (Ru/Co-Sm2O3) on H2 evolution from NaBH4 hydrolysis. Strategic annealing at 800 °C induces cobalt vacancies on the Ru/Co-Sm2O3 surface, optimizing the exposure of active sites and amplifying mass-charge transfer efficiency. Consequently, the defect-enriched Ru/Co-Sm2O3 showcases an impressive hydrogen generation rate (HGR = 0.430 mol min−1 gcatalyst−1) and outstanding cycling resilience, eclipsing the performance of most contemporary catalysts. Experimental findings reveal that Sm can not only adjust the Ru lattice spacing to accommodate more BH4−, but also modulate the Co vacancy concentration, thus bolstering the charge transport and ameliorating the catalyst's electrical conductivity. DFT calculations confirm that the Michaelis-Menten/Eley-Rideal mechanism is more appropriate to explain the hydrolysis of NaBH4.