Atomically precise Ni6(SC2H4Ph)12 nanoclusters on graphitic carbon nitride nanosheets for boosting photocatalytic hydrogen evolution

Much effort has been devoted to improving the photocatalytic capacity of graphitic carbon nitride (g-C3N4). In this paper, we reported the successful synthesis of a hybrid photocatalyst with superb photocatalytic hydrogen production activity through decorating atomically precise Ni6(SC2H4Ph)12 nanoclusters on g-C3N4 nanosheets (labeled as Ni6/g-C3N4) at room temperature. Zeta potential experiments demonstrated that the electrostatic interaction between Ni6 and g-C3N4 led to the formation of Ni6/g-C3N4. The photocatalytic measurements revealed that the 5 %-Ni6/g-C3N4 prepared with the original mass ratio of m(Ni6)/m(g-C3N4) = 1/20 exhibited the strongest hydrogen production activity. In the system with triethanolamine (TEOA) as the sacrifice agent, the visible-light hydrogen production rate reached up to 5.87 mmol h-1 g-1, approximately 290 times higher than that of pure g-C3N4 (0.02 mmol h-1 g-1). Density functional theory (DFT) calculations testified that the above significant enhancement of photocatalytic hydrogen evolution of the hybrid photocatalyst arose from the photogenerated electrons transfer from Ni6 to g-C3N4.