Study on the catalytic mechanism of core-shell structure CoCu@BN promoting the hydrolytic dehydrogenation of ammonia borane

Ammonia borane (NH 3 BH 3 , AB) as one of the complex hydrides shows great potential for hydrogen storage. Nevertheless, the lack of efficient catalysts limits the hydrogen release rate. Herein, we reported a heterostructure catalyst consisting of Co and Cu nanoparticles with a boron nitride cladding (defined as CoCu@BN). Remarkably, on the basis of BN shell formation, CoCu particles are confined with a stable nanoscale of around 10 nm. As a result, the optimal Co 0 8 Cu 0.2 @BN catalyst demonstrates excellent catalytic performance, achieving a high TOF of 28.8 mol H2 mol metal −1 min −1 , which is far superior to the Co@BN and Cu@BN. The catalytic mechanism has been verified, demonstrating that the combined compositional and structural characteristics of Co 0 · 8 Cu 0.2 @BN synergistically induce robust electron transfer. This phenomenon accelerates the cleavage of H 2 O molecules (the rate-determining step), thereby enhancing the catalytic hydrolysis of AB. The findings presented in this study offer a precise and controllable strategy for designing non-noble metal catalysts aimed at hydrogen production. Based on the strong CoCu interfacial effect from the heterostructure, we have demonstrated the as-synthesized Co 0 · 8 Cu 0.2 @BN exhibits superior catalytic effects with a TOF of 28.8 min −1 at 298 K, which is more than twice that of Co@BN and over 14 times higher than Cu@BN. • Cobalt and copper form a heterostructure rather than an alloy. • The Co 0 . 8 Cu 0.2 @BN catalyst has a core–shell structure with metal nanoparticles encapsulated in a 2.3 nm boron nitride shell. • The catalyst shows a markedly enhanced turnover frequency of 28.8 min −1 for ammonia borane hydrolysis, outperforming monometallic counterparts. • Its unique composition and structure promote strong electron transfer, significantly boosting catalytic performance.