Experimental and Theoretical Investigation of Ammonia Borane Dehydrogenation Using an Aniline‐Enhanced Ru Nanocatalyst

This study aimed to synthesize carbon quantum dots (CQDs) through the interaction of carboxyl (‐COOH) and amino (‐NH 2 ) groups and to investigate experimentally and theoretically hydrogen (H 2 ) production efficiency from ammonia borane (AB) hydrogen source using this CQDs structure with ruthenium (Ru) catalyst support material. CQDs were obtained by the hydrothermal method from aniline (A) and trichloroacetic acid (TCA) under weak base–acid coupling. A heterogeneous Ru@ATCA catalyst is developed using Ru metal nanoclusters decorated on CQDs. The development process is characterized by advanced analytical methods (UV, PL, BET, ICP‐OES, TEM, XPS, XRD). As a result of the AB catalytic reaction at 298 K, a very high Hydrogen Production Rate (HGR) of 102.1 L/g.min and a catalyst cycle frequency (TOF) of 356 min −1 are obtained. The reaction proceeds in a first‐order manner, with activation energy (Ea) of 22.3 kJ/mol, activation enthalpy and entropy of 19.65 and −29.95 J/mol, respectively. The mesoporous structures under this interaction, the increase in active surface area increases H 2 production efficiency by providing lower viscosity for both AB hydrolysis and the surrounding molecular groups. The H 2 production efficiency is compared with GFN1xTB modeling. According to modeling, the Ru activity of the weak acid TCA alone has a weaker catalytic effect than the Ru activity resulting from its interaction with the weak base aniline molecule, demonstrating the importance of the weak acid and weak base interactions.