Two-dimensional molybdenum boride coordinating with ruthenium nanoparticles to boost hydrogen generation from hydrolytic dehydrogenation of ammonia borane

J Colloid Interface Sci. 2024 Sep:669:794-803. doi: 10.1016/j.jcis.2024.05.020. Epub 2024 May 10.

Abstract

The coordination between carrier and active metal is critical to the catalytic efficiency of ammonia borane (AB) hydrolysis reaction. In the present study, we report a new type of catalytic support based on molybdenum boride (MBene) MoAl1-xB and demonstrate that the effective combination of MoAl1-xB with Ru nanoparticles can realize the significantly enhanced performance for hydrogen generation. Owing to the efficient activation and dissociation of reactants, the optimal Ru/MoAl1-xB catalyst achieves the large turnover frequency of 494 molH2 molRu-1 min-1, high hydrogen generation rate of 119817 mL min-1 gRu-1 and favorable apparent activation energy of 39.2 kJ mol-1 for the catalytic hydrolysis of AB under alkaline-free condition. The isotopic test suggests the cleavage of OH bond in H2O is the rate-determining step for hydrolysis reaction, while the fracture of B-H bond in AB is also well revealed by attenuated total reflectance (ATR)-Fourier transform infrared (FTIR) spectroscopy. Significantly, the flexible on-demand hydrogen generation is achieved by using chemical switches for on-off AB hydrolysis. This study provides a new support platform based on two-dimensional MBene to exploit efficient catalysts to boost AB dehydrogenation.

Keywords: Ammonia borane; Dehydrogenation; Hydrolysis; MoAl(1-x)B; Ruthenium.