Partial Sulphidation to Regulate Coordination Structure of Single Nickel Atoms on Graphitic Carbon Nitride for Efficient Solar H<sub>2</sub> Evolution
Guanchao Wang, Ying Ma, Ting Zhang, Yuefeng Liu, Baojun Wang, Riguang Zhang, Zhongkui Zhao
Abstract
Abstract To develop a non‐precious highly efficient cocatalyst to replace Pt on graphitic carbon nitride (g‐C 3 N 4 ) for solar H 2 production is great significant, but still remains a huge challenge. The emerging single‐atom catalyst presents a promising strategy for developing highly efficient non‐precious cocatalyst owing to its unique adjustability of local coordination environment and electronic structure. Herein, this work presents a facile approach to achieve single Ni sites (Ni 1 ‐N 2 S) with unique local coordination structure featuring one Ni atom coordinated with two nitrogen atoms and one sulfur atom, confirmed by high‐angle annular dark‐field scanning transmission electron microscopy, X‐ray absorption spectroscopy, and density functional theory calculation. Thanks to the unique electron structure of Ni 1 ‐N 2 S sites, the 1095 µmol g −1 h −1 of high H 2 evolution rate with 4.1% of apparent quantum yield at 420 nm are achieved. This work paves a pathway for designing a highly efficient non‐precious transition metal cocatalyst for photocatalytic H 2 evolution.