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Heterostructured Co_(3)O_(4)-SnO_(2)composites containing oxygen vacancy with high activity and recyclability toward NH_(3)BH_(3)dehydrogenation

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Rare Metals 2023年第9期42卷 3013-3023页

作者： Hui-Ze Wang You-Xiang Shao Yu-Fa Feng Yu-Jie Tan Qing-Yu Liao Xiao-Dong Chen Xue-Feng Zhang Zhao-Hui Guo Hao Li School of Chemistry and Materials Engineering Huizhou UniversityHuizhou516007China Guangdong Provincial Key Laboratory for Electronic Functional Materials and Devices Huizhou UniversityHuizhou516007China

Ammonia borane(NH_(3)BH_(3),AB)has been regarded as a promising chemical hydrogen storage material owing to its high hydrogen density and superior stability.Thus,the development of low-cost and high-efficient heterogeneous catalysts for the dehydrogenation of AB has attracted considerable scholarly attention.In this study,heterostructured Co_(3)O_(4)-SnO_(2)catalysts containing oxygen vacancy(V_(o))with different Co/Sn atomic ratios(designated as V_(o)-Co-Sn_(5:x))were synthesized via a simple coprecipitation-calcination method under mild reaction conditions.The catalyst containing an optimized Co/Sn atomic ratio of 5:2(V_(o)-Co-Sn_(5:2))exhibited robust catalytic performance with a turnover frequency value of 17.6mol_(H2)·mol^(-1)_(metal)·min^(-1).Moreover,82.6%of the original activity of the catalyst was retained after 14 catalytic cycles,indicating the high stability of the catalyst.Diversified characterization combined with the density functional theory(DFT)calculation confirmed the transfer of electrons from Co_(3)O_(4)to Sn O_(2)and the distribution of the separated charges on SnO_(2)-Co_(3)O_(4)interface.The transfer of electrons and the distribution of charges facilitated the adsorption and activation of water on the catalyst,thus accelerating the dissociation of H_(2)O molecule(the ratedetermining step of AB hydrolysis).It was found that the V_(o)adjusted the electron structure of the catalysts rather than acted as active sites.These findings will provide researchers with useful information for designing cheap and highly efficient catalysts for catalytic AB hydrolysis.

关键词： Ammonia borane(AB) cobalt-tin composite oxide Heterocatalysis Hydrogen production Oxygen vacancy

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