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

Abstract Hydrolysis of ammonia borane (NH3BH3, 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 NH3BH3 and H2O molecules on the Ru and Pt sites as well as facilitate the fast transfer of *H and the desorption of H2 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.