Nitrogen doping excited Ru and Ti3C2−xNx support for hydrogen generation from ammonia borane

The research and development of efficient catalysts is very important for the sustainable utilization of hydrogen energy. Herein, we designed the Ru/Ti 3 C 2−x N x catalysts using N -doped two-dimensional material MXene (Ti 3 C 2−x N x ) as support toward hydrogen generation from ammonia borane (AB) hydrolysis. Due to the confinement and anchoring effects of Ti 3 C 2−x N x , the as-prepared Ru/Ti 3 C 2−x N x catalysts show an ultrafine particle size of 1.55 nm and remarkable AB hydrolysis activity with high turnover frequency (TOF) value of 1334 min −1 and r B value of 297 × 10 3  mL·min −1 ·g Ru −1 at 298 K. XPS results show that the doped N atoms in Ti 3 C 2−x N x support provide electron-feeding effect for Ru in the reaction to form electron-rich Ru. The isotope experiments confirm that the dissociation of H 2 O is the rate-determining step (RDS) in AB hydrolysis reaction catalyzed by Ru/Ti 3 C 2−x N x . According to the density functional theory (DFT) calculations, the N atoms introduced into Ti 3 C 2−x N x decrease the dissociation energy of O–H bond in H 2 O molecules, accelerating the desorption of H* from Ti 3 C 2−x N x surface. This research provides a strategy to enhance synergistic interaction between support and metal through N -doping, so as to effectively improve the catalytic performance of heterogeneous catalysts.