3D-Cobalt-Dicyanamide-Derived 2D-Layered-Co(OH)₂-Based Catalyst for Light-Driven Hydrogen Evolution

Derivation of 3D coordination polymers to produce active catalysts has been a feasible strategy to achieve a precise coordination sphere for the catalytic site. This study demonstrates the partial conversion of a 3D cobalt dicyanamide coordination polymer, Co-dca, to a 2D layered hydroxide-oxyhydroxide structure under photocatalytic conditions. The catalyst exhibits an activity as high as 28.3 mmol h(-1) g(-1) in the presence of a [Ru(bpy)(3)](2+)/triethylamine (TEA) couple to maintain it for at least 12 h. Photocatalytic and characterization studies reveal that the dicyanamide ligand within the coordination polymer is crucial for governing modification and achieving a superior H-2 evolution rate. Moreover, we observed the critical role of TEA as the hydrolyzing agent for the transformation process. This study displays that the metal dicyanamides can be utilized as templates for preparing active and robust catalysts.