Adaptive Coordination Engineering for Efficient and Robust H₂ Release

Efficient regulation of β-H activation and its subsequent elimination remains a notorious challenge owing to stringent inherent geometric and electronic constraints. To overcome the high kinetic barriers, it necessitates a precise catalyst to effectively orchestrate the metal-substrate interaction. Herein, we report a molecular Pd₁-Ag₂ model using a tridentate phosphine ligand (L2) and formate bridges, which integrates the effect of double silver synergy and nitrate anion regulation, and serves as the core origin to facilitate efficient β-H elimination. Such bimetallic cooperation optimizes the reaction pathway and realizes rapid hydrogen production with complete CO-free characteristics, endowing prominent industrial advantages over monometallic counterparts. Under ambient air at 60°C, this catalyst delivers excellent activity and satisfactory recyclability. DFT calculations confirm that the rate-determining β-H elimination step of monometallic Pd systems is effectively optimized, and in situ spectroscopic measurements further verify the stable proximal Pd-Ag synergistic coordination throughout the reaction.