H2 generation from catalytic water dissociation on doped nanocluster Pt6X (X=C, Si, and Ge)

Noble-metal nanoclusters, as catalysts, are attracting increasingly significant attention due to abundant active electrons and diversity of properties. However, reaction by-products always adhere to the catalytic clusters and prevent redox reactions. Doping earth-abundant elements to form alloy can lower the material cost and improve the electrochemical characters to overcome the “catalyst poisoning”. Herein, we investigated the effects of doping a carbon-group element (X = C, Si, or Ge) atom in a Pt7 cluster, forming a Pt6X cluster, by density functional theory calculations. Based on the reaction coordinate analysis, we found that the Pt6X cluster is superior to the Pt7 cluster in catalytic activity of water dissociation. Our findings show that introducing heteroatoms can efficiently enhance the charge accepting ability and evoke active sites, thus improving the catalytic hydrogen extraction from H2O, which provide meaningful insights into the alloy nanoparticle catalysts.