Single-Atom Catalysis for CO Combustion in Automotive Exhaust: A DFT Study

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-03-07 DOI:10.1007/s10562-025-04983-0

Li Cai, Chunlan Qin, Lidong Zhang

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Abstract

Automotive emissions, particularly carbon monoxide (CO), are a significant environmental concern, and effective catalytic solutions for their treatment are critical for reducing air pollution. Regulating different coordination environments to enhance the catalytic combustion activity of CO on cobalt graphene single-atom catalysts (CoNx-Gr) is an effective method. The possible reaction mechanism pathways of CO on CoNx-Gr were systematically studied through theoretical calculations. By comparing the energy distribution of three mechanisms, the best coordination environment catalyst was screened out, which is the tri-nitrogen coordination with an energy barrier of only 0.40 eV. Compared to the Eley–Rideal (ER) mechanism, CoNx-Gr dominated by the Termolecular Eley–Rideal (TER) mechanism still exhibits high catalytic combustion performance for CO at room temperature. The stability of the CoNx-Gr catalyst was verified through cohesive energy and ab initio molecular dynamics (AIMD) simulations. Microkinetic analysis indicates that increasing the temperature can accelerate the reaction. This work provides valuable theoretical guidance for the design of transition metal single-atom catalysts and contributes to establishing a preliminary catalytic combustion reaction kinetic model.

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.