First principles studies combined with the microkinetic analysis were performed to study the reliability and reaction mechanisms of single-atom-doped graphene materials in catalyzing NO_x reduction with CO. By screening the 3d transition metals (Sc-Zn) and group IV elements (Si and Ge), it was found that the Ti- and Co-doped graphene sheets (TiGr and CoGr), respectively, exhibited excellent catalytic activities in the NO/NO₂-to-N₂O and the N₂O-to-N₂ processes at a relatively low temperature (450 K). Therefore, the tandem catalyst (TiGr + CoGr) can be a promising catalyst in NO_x reduction with CO. It was further revealed that the combination of adsorption energy and electronegativity was a good descriptor to predict the activation energies. The obtained results provide useful information for rational design of carbon-based single-atom catalysts for NO_x reduction by CO at low temperatures.

中文翻译：

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CO 还原 NOx 能否在低温下在碳基单原子催化剂上反应？理论研究

第一原理研究与microkinetic分析相结合进行研究单原子掺杂的石墨烯材料的可靠性和反应机制催化NO _X还原CO。通过筛选所述3d过渡金属（SC-Zn系）和组IV族元素（硅和 Ge），发现 Ti 和 Co 掺杂的石墨烯片（TiGr 和 CoGr）分别在 NO/NO ₂ -to-N ₂ O 和 N ₂ O-to-N 中表现出优异的催化活性₂过程在相对较低的温度 (450 K) 下进行。因此，串联催化剂（TiGr + CoGr）是一种很有前景的 NO _x催化剂。进一步表明吸附能和电负性的组合是预测活化能的良好描述。获得的结果为合理设计碳基单原子催化剂在低温下通过 CO 还原NO _x提供了有用的信息。