Preparation of highly dispersed Ni single-atom doped ultrathin g-C₃N₄ nanosheets by metal vapor exfoliation for efficient photocatalytic CO₂ reduction

Single-atom photocatalysts can modulate the utilization of photons and facilitate the migration of photogenerated carriers. However, the preparation of single-atom uniformly doped photocatalysts is still a challenging topic. Herein, we propose the preparation of Ni single-atom doped g-C3N4 photocatalysts by metal vapor exfoliation. The Ni vapor produced by calcining nickel foam at high temperature accumulates in between g-C3N4 layers and poses a certain vapor pressure to destroy the interlayer van der Waals forces of g-C3N4. Individual metal atoms are doped into the structure while exfoliating g-C3N4 into nanosheets by metal vapor. Upon optimization of Ni content, the Ni single atom doped g-C3N4 nanosheets with 2.81 wt% Ni exhibits the highest CO2 reduction performance in the absence of sacrificial agents. The generation rates of CO and CH4 are 19.85 and 1.73 mu mol g(-1)h(-1), respectively. The improved photocatalytic performance is attributed to the anchoring Ni of single atoms on g-C3N4 nanosheets, which increases both carrier separation efficiency and reaction sites. This work provides insight into the design of photocatalysts with highly dispersed single-atom.