A Promoted Charge Separation/Transfer System from Cu Single Atoms and C 3 N 4 Layers for Efficient Photocatalysis

作者：Xudong Xiao, Yanting Gao, Liping Zhang, Jiachen Zhang, Qun Zhang, Qi Li, Hongliang Bao, Jing Zhou, Shu Miao, Ning Chen, Jian‐Qiang Wang, Baojiang Jiang, Chungui Tian, Honggang Fu · 发表于：Advanced Materials · 年份：2020 · DOI：10.1002/adma.202003082 · 被引用次数：537 · 研究领域：Advanced Photocatalysis Techniques、Copper-based nanomaterials and applications、ZnO doping and properties

Abstract Establishing highly effective charge transfer channels in carbon nitride (C 3 N 4 ) for enhancing its photocatalytic activity is still a challenging issue. Herein, for the first time, the engineering of C 3 N 4 layers with single‐atom Cu bonded with compositional N (CuN x ) is demonstrated to address this challenge. The CuN x is formed by intercalation of chlorophyll sodium copper salt into a melamine‐based supramolecular precursor followed by controlled pyrolysis. Two groups of CuN x are identified: in one group each of Cu atoms is bonded with three in‐plane N atoms, while in the other group each of Cu atoms is bonded with four N atoms of two neighboring C 3 N 4 layers, thus forming both in‐plane and interlayer charge transfer channels. Importantly, ultrafast spectroscopy has further proved that CuN x can greatly improve in‐plane and interlayer separation/transfer of charge carriers and in turn boost the photocatalytic efficiency. Consequently, the catalyst exhibits a superior visible‐light photocatalytic hydrogen production rate (≈212 µmol h −1 /0.02 g catalyst), 30 times higher than that of bulk C 3 N 4 . Moreover, it leads to an outstanding conversion rate (92.3%) and selectivity (99.9%) for the oxidation of benzene under visible light.