Monodisperse Ni-clusters anchored on carbon nitride for efficient photocatalytic hydrogen evolution

The active sites of monodisperse transition metal Ni-clusters were anchored on carbon nitride (CN) by an in situ photoreduction deposition method to promote the efficient separation of photogenerated charges and achieve high-efficiency photocatalytic activity for hydrogen evolution. The Ni-cluster/CN exhibited a photocatalytic hydrogen production rate of 16.5 mmol·h–1·g–1 and a total turnover frequency (TOF (H2)) value of 461.14 h–1. X-ray absorption spectroscopy based on synchrotron radiation indicated that CN had two reaction centers to form stable interface interactions with monodispersed Ni-clusters, in which carbon can act as an electron acceptor, while nitrogen can act as an electron donor. Meanwhile, the hybrid electronic structure of the Ni-cluster/CN system was constructed, which was favorable for photocatalytic activity for hydrogen production. An in-depth understanding of the interfacial interaction between CN and Ni-clusters will have important reference significance on the mechanistic study of development based on the cocatalyst. © 2022 Dalian Institute of Chemical Physics, the Chinese Academy of Sciences