Remarkably boosting Ru-Ni nanocatalysis via surface/interface regulation for efficient hydrolytic dehydrogenation of ammonia borane

Abstract

Ammonia borane (NH3BH3, AB) has been considered as one of the most attractive candidates for chemical hydrogen-storage materials. Development of low-cost and high-performance catalysts for hydrogen generation from AB is highly desirable, which is still a huge challenge. Herein, Ru-Ni bimetallic nanoparticles were fabricated on (3-aminopropyl) triethoxysilane-functionalized reduced graphene oxide nanosheet (APTS-rGO) by a facile one-step in situ co-reduction strategy. The newly developed Ru1Ni4/APTS-rGO catalyst with hydrophilic interface and narrow particle size-distribution presented a remarkably enhanced catalytic activity for hydrolytic H2 generation from AB, affording an ultra-high TOF value of 1559 min−1. The APTS-rGO support was effective to minimize the aggregation of Ru-Ni nanoparticles, achieving the immobilization of ultrasmall Ru-Ni nanoparticles (2.0 nm) on support surface. The change in local charge density of catalyst surface caused by Ru-Ni synergistic effect and metals-support interaction improved the catalytic performance of Ru1Ni4/APTS-rGO. Hydrophilic NH2-containing interface ensured high dispersibility of catalysts in reaction solution, increasing the contact opportunities between active sites and AB molecules. These factors contributed together to the exceptional catalytic performance of Ru1Ni4/APTS-rGO. This catalytic system has potential applications in various catalytic fields due to its obvious advantages of the facile preparation method, good hydrophilicity, and the outstanding catalytic performance.