Theoretical investigation of chemical reaction kinetics of CO2 and vinyl radical under catalytic combustion. (1st December 2021)

• Record Type: Journal Article
• Authors: Ao, Chengcheng; Ruan, Shanshan; He, Wei; He, Chenliang; Xu, Kangwei; Zhang, Lidong
• Is Part Of: Fuel. Volume 305(2021)
• Publication Date: 2021-12-01
• Subjects: Carbon dioxide -- Vinyl radical -- Catalytic combustion -- DFT; Fuel -- Periodicals; Coal -- Periodicals; Coal; Fuel; Periodicals; 662.6
• DOI: 10.1016/j.fuel.2021.121566
• Languages: English
• ISSNs: 0016-2361

Abstract

Highlights: The PESs of chemical reaction of CO2 and C2 H3 under catalytic combustion are obtained using DFT method. Compared with gas-phase reaction, the energy barrier of CH2 CHO and CO formation on Pd(1 0 0) is reduced. The kinetic parameters of reaction CO2 + C2 H3 on Pd(1 0 0) are obtained based on transition state theory. Abstract: Catalytic combustion is a promising technology to improve combustion efficiency and reduce environmental pollutions. Both CO2 and vinyl radical (C2 H3 ) are important species and give rise to environmental concerns. It is meaningful to investigate the combustion reaction CO2 + C2 H3 under catalytic combustion, which helps to mitigate environmental damage. In this context, the theoretical study of chemical reaction kinetics of CO2 and C2 H3 on Pd(1 0 0) and Cu(1 0 0) was carried out. Compared with conventional gas-phase combustion reaction, catalytic combustion has only two reaction paths, producing CO + CH2 CHO and C2 H2 + OCHO, respectively. The catalysts show superior performance in decomposition reactions, with Pd(1 0 0) in particular greatly reducing the energy barrier for the formation of CO + CH2 CHO. And Pd(1 0 0) is preferred to form CO and CH2 CHO rather than C2 H2 and OCHO which are favorable in gas-phase reaction. In addition, the kinetic parameters of reaction CO2 + C2 H3 on Pd(1 0 0) are obtained based on transition state theory. The results indicate that the formation of CH2 CHO and CO dominates the reaction CO2 + C2 H3 . This work investigates the mechanism of reaction of CO2 and C2 H3 on Pd(1 0 0) and Cu(1 0 0), paving the way for further research on the catalytic combustion mechanism and the regulation of pollutant emissions.