Citation: Shao-Hua LIU, Yi LI, Kai-Ning DING, Wen-Kai CHEN, Yong-Fan ZHANG, Wei LIN. Mechanism on Carbon Vacancies in Polymeric Carbon Nitride for CO₂ Photoreduction[J]. Chinese Journal of Structural Chemistry, ;2020, 39(12): 2068-2076. doi: 10.14102/j.cnki.0254–5861.2011–3005 shu

Mechanism on Carbon Vacancies in Polymeric Carbon Nitride for CO₂ Photoreduction

Shao-Hua LIU ^a ,
Yi LI ^{a, b} ,
Kai-Ning DING ^a ,
Wen-Kai CHEN ^{a, b} ,
Yong-Fan ZHANG ^{a, b} ,
Wei LIN ^{a, b,,}

a.
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350108, China
b.
Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, Xiamen 361005, China

Corresponding author: Wei LIN, wlin@fzu.edu.cn
Received Date: 22 October 2020
Accepted Date: 17 November 2020

Fund Project: the National Natural Science Foundation of China 21973014the National Natural Science Foundation of China 21773030

Figures(7)

Defect engineering has being regarded as one of the effective ways to regulate chemical and electronic structure of semiconductors. Recently, our collaborative work has shown experimentally that carbon vacancy on polymeric carbon nitride (CV) can greatly improve the CO₂ to CO conversion with a 45-fold improvement over the polymeric carbon nitride (Angew. Chem. Int. Ed., 2019, 58, 1134). In order to clarify the detailed mechanism of promotion, we have systematically studied the electronic properties of CV and hydrogenated CV (CV_+H) as well as the effective CO₂ reduction reaction through density functional theory calculations. We found that it is the synergistic effect for the CO₂ reduction reaction in the CV systems, as the onset potentials of several CVs are much lower than that of the polymeric carbon nitride. In particular, the onset potentials of CV₁, CV₂, and CV_2+H are around 0.9~1.5 eV with a strong chemisorbed CO₂ on them. Combined with the analysis of the electronic properties, our results confirm that defect engineering increases the lifetime of photo-generated charges, improves photocatalytic activity, and promotes the CO₂ reduction reaction on the defected polymeric carbon nitrides.
- polymeric carbon nitride (PCN),
- carbon vacancy,
- reaction mechanism,
- CO₂ reduction,
- density functional theory (DFT)
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Mechanism on Carbon Vacancies in Polymeric Carbon Nitride for CO2 Photoreduction

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通讯作者: 陈斌, bchen63@163.com

Mechanism on Carbon Vacancies in Polymeric Carbon Nitride for CO₂ Photoreduction