Synergizing Mg Single Atoms and Ru Nanoclusters for Boosting the Ammonia Borane Hydrolysis to Produce Hydrogen.

Development of efficient catalysts with high H2O molecule activation ability holds great importance for H2 production. Herein, enzyme‐mimic Mg single atoms catalysts (SACs) coordinated by B/N‐doped carbon nanotube (BNC), was constructed as a high‐performance support for ruthenium (Ru) nano‐clusters. Dual functions of Mg SACs were discovered, where the Mg atoms beneath Ru catalysts built an interfacial electron polarization, inducing electron transfer from Ru to the Mg‐BNC support. In addition, the oxyphilic Mg SACs adjacent to the Ru catalysts could actively participate in H2O adsorption. The combination of experimental characterization, reaction kinetics study and density functional theory (DFT) calculations validated a stronger intrinsic H2O activation capability at the positive Ru sites. Meanwhile, the synergistic Mg SACs jointly contribute to the acceleration of the sluggish H2O dissociation process in ammonia borane (AB) hydrolysis reaction, resulting in exceptional hydrogen production activity and catalytic stability, outperforming most state‐of‐the‐art Ru‐based catalysts. This work provides a new strategy for utilizing alkaline earth metals as both the electronic promoter and the reactant activator, offering inspiration for the development of advanced heterogeneous catalysts. [ABSTRACT FROM AUTHOR]