Harmful carbon monoxide (CO) gas from vehicle exhaust and fossil fuel combustion seriously affects the ecological environment and human health, although this issue can be effectively solved by low-temperature catalytic combustion. Herein, an Fe and N codoped double vacancy graphene catalyst (Fe-CxNy) for the low-temperature catalytic combustion of CO is proposed, and the mechanism of the CO catalytic combustion reaction over the catalyst is systematically investigated by using density function theory (DFT). Four oxidation mechanisms, including Eley–Rideal (ER1 and ER2), Langmuir-Hinshelwood (LH) and Termolecular Eley–Rideal (TER), were compared in terms of oxidation pathways and energy distribution. All the results indicate that Fe-CxNy catalysts have efficient catalytic activity. The Fe-CN₃ catalyst with the predominant LH reaction mechanism showed the best performance for the catalytic combustion of CO with only 0.20 eV, which was comparable to that of noble metals. The rate constant calculations further demonstrate that Fe-CN₃ exhibits excellent catalytic performance at low temperatures. This work not only provides a theoretical basis for the design and development of low-temperature catalytic combustion CO catalysts, but also provides data support for the kinetic model of CO combustion reaction.

汽车尾气和化石燃料燃烧产生的有害一氧化碳（CO）气体严重影响生态环境和人体健康，低温催化燃烧可以有效解决这一问题。在此，提出了一种用于 CO 低温催化燃烧的 Fe 和 N 共掺杂双空位石墨烯催化剂（Fe-CxNy），并利用密度泛函理论（DFT）系统地研究了催化剂上 CO 催化燃烧反应的机理). 在氧化途径和能量分布方面比较了四种氧化机制，包括 Eley–Rideal（ER1 和 ER2）、Langmuir-Hinshelwood (LH) 和 Termolecular Eley–Rideal (TER)。所有结果表明Fe-CxNy催化剂具有高效的催化活性。Fe-CN ₃LH 反应机制占主导地位的催化剂对 CO 的催化燃烧表现出最佳性能，仅为 0.20 eV，与贵金属相当。速率常数的计算进一步表明Fe-CN ₃在低温下表现出优异的催化性能。该工作不仅为低温催化燃烧CO催化剂的设计和开发提供了理论依据，也为CO燃烧反应的动力学模型提供了数据支持。