Abstract Metal-free catalysts for the CO2 reduction reaction (CO2RR) is a research hotspot to enhance CO2 utilization as a way to counteract global warming. Nitrogen-doped graphene attracts attention because of the abundance of nitrogen and promising catalytic performance of graphene. In this work, we investigated various N-doped configurations and their corresponding catalytic abilities for CO2RR to ethanol via spin-polarized density functional theory (DFT) computations. The final results indicate that site 43 of binary-N-doped graphene had high CO2RR activity, stable adsorption of reactants, and good activation of CO2. The catalysis process demonstrated features of low free energy barriers in the rising stage and obvious facilitation of the potential-limiting step. Compared with a catalyst-free process, it can effectively improve the reaction activity. The results provide theoretical guidance for the design and preparation of high-performance CO2RR catalysts.

中文翻译：

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氮掺杂石墨烯作为 CO2RR 高性能电催化剂的密度泛函理论研究

摘要 用于二氧化碳还原反应（CO2RR）的无金属催化剂是提高二氧化碳利用率以应对全球变暖的研究热点。氮掺杂石墨烯因其丰富的氮和石墨烯的催化性能而备受关注。在这项工作中，我们通过自旋极化密度泛函理论 (DFT) 计算研究了各种 N 掺杂配置及其相应的 CO2RR 到乙醇的催化能力。最终结果表明，二元氮掺杂石墨烯的 43 位点具有较高的 CO2RR 活性、稳定的反应物吸附和良好的 CO2 活化。催化过程表现出上升阶段自由能垒低和限位步骤明显促进的特点。与无催化剂工艺相比，能有效提高反应活性。研究结果为高性能CO2RR催化剂的设计和制备提供了理论指导。