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Ammonia borane methanolysis for hydrogen evolution on Cu3Mo2O9/NiMoO4 hollow microspheres

Jinyun Liao,Yujie Wu,Youxiang Shao,Yufa Feng,Xuefeng Zhang,Wanling Zhang,Junhao Li,Ming Wu,Huafeng Dong,Quanbing Liu,Hao Li

Catalytic methanolysis of ammonia borane (AB) is an integrated hydrogen storage-production technology with bright prospects; the development of robust and cheap catalysts is crucial for its wide applications. In this study, we developed heterostructured Cu 3 Mo 2 O 9 /NiMoO 4 hollow spheres comprised of nanoplatelets as catalysts for AB methanolysis. The Cu 3 Mo 2 O 9 /NiMoO 4 catalyst with the optimal Cu/Ni ratio exhibited robust reactivity with a turnover frequency (TOF) of 62.1 mol hydrogen min −1 mol cat −1 , which is superior to other precious-metal-free catalysts ever reported in the literature. Based on the theoretical calculation results, it was found that the d band center of the heterostructured Cu 3 Mo 2 O 9 /NiMoO 4 catalysts exhibited an up shift compared to those of single Cu 3 Mo 2 O 9 and NiMoO 4 , which was favorable for the chemisorption of the reactants. In addition, it was revealed that the active Ni and Cu sites in Cu 3 Mo 2 O 9 /NiMoO 4 catalysts were responsible for the adsorption and activation of CH 3 OH and AB, respectively. The rate-determining step of AB methanolysis over Cu 3 Mo 2 O 9 /NiMoO 4 catalyst was identified, and a possible reaction mechanism was proposed. This study may provide a deeper understanding of the adsorption and activation behaviors of methanol and AB, cooperative roles of different active sites on the heterostructured catalyst, as well as the reaction mechanism, conducive to the rational design of inexpensive and high-performing catalysts for AB methanolysis for hydrogen production.