Anchoring Single Nickel Atoms on Carbon-vacant Carbon Nitride Nanosheets for Efficient Photocatalytic Hydrogen Evolution

摘要

Polymeric carbon nitride(PCN)has emerged as a promising candidate for photocatalytic hydrogen evolution,but its dependence on scarce and high-cost noble metal co-catalysts severely limits its extensive application.It will be of great promise to develop non-noble metal single-atom co-catalysts with low-cost and high atom utilization to improve the photocatalytic performance over PCN.Herein,single Ni atoms are successfully anchored onto carbon-vacant PCN nanosheets(CCN-SANi)via a two-step ammonia thermal treatment and photo-deposition process.Theoretical calculations and experimental results demonstrate that the optical absorption property and the charge transfer ability of CCN-SANi have been significantly improved with the introduction of single Ni atoms to form Ni-N3 sites.In comparison to carbon-vacant PCN(CCN)loaded with Ni clusters,the obtained CCN-SANi exhibits 11.4 times increased photocatalytic performance,with the highest hydrogen evolution rate reaching 511μmol/(g·h),which is even 1.7 times higher than that of CCN loaded with Pt clusters.This research proposes an inspiring and reliable strategy to design novel single-atom semiconducting polymers with electronic structures manipulated for efficient photocatalysis.