Stable single iron atom within two-dimensional porphyrin sheet catalysis for CO oxidation: A computational investigation. (15th June 2023)

• Record Type: Journal Article
• Authors: Xie, Kefeng; Xu, Shengyuan; Xu, Kai; Wang, Jie; Ma, Longjun; Lin, Jun-Bing
• Is Part Of: Fuel. Volume 342(2023)
• Publication Date: 2023-06-15
• Subjects: CO oxidation -- Single-atom catalysts -- Two-dimensional porphyrin sheet -- Iron atom; Fuel -- Periodicals; Coal -- Periodicals; Coal; Fuel; Periodicals; 662.6
• DOI: 10.1016/j.fuel.2023.127890
• Languages: English
• ISSNs: 0016-2361

Abstract

Graphical abstract: Highlights: The mechanism of CO oxidation on two-dimensional porphyrin sheet with single iron atom was investigated by density functional theory. The current results indicated that two-dimensional porphyrin sheet with single iron atom was a candidate catalyst for CO oxidation under mild conditions, providing an excellent substrate for single-atom catalysts. Abstract: CO produced by incomplete combustion of fuel poses a great threat to the environment and human health. Single atom catalysis can increase the active site of the catalyst, but it is unstable and easy to agglomerate at the higher temperatures. A stable single iron atom two-dimensional porphyrin sheet (Fe–TDPS) was designed, which was as CO oxidation catalyst to reduce costs and increase catalytic activity, and the reaction mechanism was investigated by density functional theory. Fe–TDPS has good stability at 1000 K with the ab initio molecular dynamics simulation. Absorption energies suggested that both CO and O2 preferred to anchor at the Fe–N4 site. The mechanisms of CO oxidation, which have reacted on the Fe–TDPS, were explored by Langmuir–Hinshelwood, Eley–Rideal, and ter-molecular Eley–Rideal mechanisms. Ter-molecular Eley–Rideal mechanism was feasible because of the small energy barrier. Results indicated that Fe–TDPS can be used as a catalyst for CO oxidation in the mild condition.