Partial Sulphidation to Regulate Coordination Structure of Single Nickel Atoms on Graphitic Carbon Nitride for Efficient Solar H2 Evolution

• Published in: Small (Weinheim an der Bergstrasse, Germany) Germany), 2023-02, Vol.19 (6), p.e2205758-n/a
• Main Authors: Wang, Guanchao, Ma, Ying, Zhang, Ting, Liu, Yuefeng, Wang, Baojun, Zhang, Riguang, Zhao, Zhongkui
• Format: Article
• Language: English
• Subjects: Absorption spectroscopy; Carbon; Carbon nitride; Coordination; Density functional theory; Electronic structure; graphitic carbon nitride; Hydrogen evolution; Hydrogen production; local electronic structure regulation; Nanotechnology; Nickel; Nitrogen atoms; nonprecious single atom cocatalysts; photocatalysis; Scanning transmission electron microscopy; Sulfidation; Transition metals
• ISSN: 1613-6810; 1613-6829
• DOI: 10.1002/smll.202205758

To develop a non‐precious highly efficient cocatalyst to replace Pt on graphitic carbon nitride (g‐C3N4) for solar H2 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 (Ni1‐N2S) 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 Ni1‐N2S sites, the 1095 µmol g−1 h−1 of high H2 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 H2 evolution. This work reports the unique single Ni sites (Ni1‐N2S) on graphitic carbon nitride with unique local coordination structure featuring one Ni atom coordinated with two nitrogen atoms and one sulfur atom, acting as non‐precious metal cocatalyt to efficiently promote H2 evolution from water splitting under visible light irradiation, ascribed to the unique electron structure of Ni1‐N2S sites.