Crystalline Carbon Nitride Supported Copper Single Atoms for Photocatalytic CO2 Reduction with Nearly 100% CO Selectivity

光催化 材料科学 无定形固体 催化作用 氮化碳 金属 纳米棒 无定形碳 化学工程 无机化学 吸附 纳米技术 物理化学 结晶学 化学 冶金 有机化学 工程类
作者
Yang Li,Baihai Li,Dainan Zhang,Lei Cheng,Quanjun Xiang
出处
期刊:ACS Nano [American Chemical Society]
卷期号:14 (8): 10552-10561 被引量:563
标识
DOI:10.1021/acsnano.0c04544
摘要

Single metal atom photocatalysts have received widespread attention due to the rational use of metal resources and maximum atom utilization efficiency. In particular, N-rich amorphous g-C3N4 is always used as a support to anchor single metal atoms. However, the enhancement of photocatalytic activity of g-C3N4 by introducing a single atom is limited due to the bulk morphology and the excess defects of amorphous g-C3N4. Here, we report crystalline g-C3N4 nanorod supported copper single atoms by molten salts and the reflux method. The prepared single Cu atoms/crystalline g-C3N4 photocatalyst (Cu-CCN) shows highly selective and efficient photocatalytic reduction of CO2 under the absence of any cocatalyst or sacrificial agent. The introduction of single Cu atoms can be used as the CO2 adsorption site, thus increasing the adsorption capacity of Cu-CCN samples to CO2. Theoretical calculation results show that reducing CO2 to CH4 on Cu-CCN samples is an entropy-increasing process, whereas reducing CO2 to CO is an entropy-decreasing process. As a result, the Cu-CCN samples exhibited enhanced photocatalytic CO2 reduction with nearly 100% selective photocatalytic CO2 to CO conversion. The mechanism of photocatalytic CO2 reduction over Cu-CCN samples was proposed based on in situ Fourier transform infrared spectra, X-ray absorption spectroscopy, and density functional theory calculation. This work provides an in-depth understanding of the design of photocatalysts for enhancing active sites of the reactants.
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