Efficient Hydrogen Generation from Ammonia Borane Hydrolysis on a Tandem Ruthenium-Platinum-Titanium Catalyst.

Hydrolysis of ammonia borane (NH 3 BH 3 , AB) involves multiple undefined steps and complex adsorption and activation, so single or dual sites are not enough to rapidly achieve the multi-step catalytic processes. Designing multi-site catalysts is necessary to enhance the catalytic performance of AB hydrolysis reactions but revealing the matching reaction mechanisms of AB hydrolysis is a great challenge. In this work, we propose to construct RuPt-Ti multi-site catalysts to clarify the multi-site tandem activation mechanism of AB hydrolysis. Experimental and theoretical studies reveal that the multi-site tandem mode can respectively promote the activation of NH 3 BH 3 and H 2 O molecules on the Ru and Pt sites as well as facilitate the fast transfer of *H and the desorption of H 2 on Ti sites at the same time. RuPt-Ti multi-site catalysts exhibit the highest turnover frequency (TOF) of 1293 min -1 for AB hydrolysis reaction, outperforming the single-site Ru, dual-site RuPt and Ru-Ti catalysts. This study proposes a multi-site tandem concept for accelerating the dehydrogenation of hydrogen storage material, aiming to contribute to the development of cleaner, low-carbon, and high-performance hydrogen production systems.