Efficient catalytic oxidation of formaldehyde by defective g-C 3 N 4 -anchored single-atom Pt: A DFT study.

Autor: Zheng Z; State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China., Zhang C; State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China. Electronic address: chengzhang@hust.edu.cn., Li J; State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China., Fang D; State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China., Tan P; State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China., Fang Q; State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China., Chen G; State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China.
Jazyk: angličtina
Zdroj: Chemosphere [Chemosphere] 2024 Aug; Vol. 361, pp. 142517. Date of Electronic Publication: 2024 Jun 01.
DOI: 10.1016/j.chemosphere.2024.142517
Abstrakt: Indoor volatile formaldehyde is a serious health hazard. The development of low-temperature and efficient nonhomogeneous oxidation catalysts is crucial for protecting human health and the environment but is also quite challenging. Single-atom catalysts (SACs) with active centers and coordination environments that are precisely tunable at the atomic level exhibit excellent catalytic activity in many catalytic fields. Among two-dimensional materials, the nonmagnetic monolayer material g-C 3 N 4 may be a good platform for loading single atoms. In this study, the effect of nitrogen defect formation on the charge distribution of g-C 3 N 4 is discussed in detail using density functional theory (DFT) calculations. The effect of nitrogen defects on the activated molecular oxygen of Pt/C 3 N 4 was systematically revealed by DFT calculations in combination with molecular orbital theory. Two typical reaction mechanisms for the catalytic oxidation of formaldehyde were proposed based on the Eley-Rideal (E-R) mechanism. Pt/C 3 N 4 -V 3N was more advantageous for path 1, as determined by the activation energy barrier of the rate-determining step and product desorption. Finally, the active centers and chemical structures of Pt/C 3 N 4 and Pt/C 3 N 4 -V 3N were verified to have good stability at 375 K by determination of the migration energy barriers and ab initio molecular dynamics simulations. Therefore, the formation of N defects can effectively anchor single-atom Pt and provide additional active sites, which in turn activate molecular oxygen to efficiently catalyze the oxidation of formaldehyde. This study provides a better understanding of the mechanism of formaldehyde oxidation by single-atom Pt catalysts and a new idea for the development of Pt as well as other metal-based single-atom oxidation catalysts.
Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests:Cheng Zhang reports was provided by National Natural Science Foundation of China. Cheng Zhang reports a relationship with Huazhong University of Science and Technology that includes: non-financial support. nothing If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
(Copyright © 2024 Elsevier Ltd. All rights reserved.)
Databáze: MEDLINE
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