Electrochemical reduction of CO₂ to chemical fuel offers a promising strategy for managing the global carbon balance, but presents challenges for chemistry due to the lack of effective electrocatalyst. Here we report atomically dispersed nickel on nitrogenated graphene as an efficient and durable electrocatalyst for CO₂ reduction. Based on operando X-ray absorption and photoelectron spectroscopy measurements, the monovalent Ni(i) atomic center with a d⁹ electronic configuration was identified as the catalytically active site. The single-Ni-atom catalyst exhibits high intrinsic CO₂ reduction activity, reaching a specific current of 350 A g_catalyst⁻¹ and turnover frequency of 14,800 h⁻¹ at a mild overpotential of 0.61 V for CO conversion with 97% Faradaic efficiency. The catalyst maintained 98% of its initial activity after 100 h of continuous reaction at CO formation current densities as high as 22 mA cm⁻².

用电化学方法将CO ₂还原为化学燃料为管理全球碳平衡提供了一种有前途的策略，但由于缺乏有效的电催化剂，因此在化学方面面临挑战。在这里，我们报告原子分散在氮化石墨烯上的镍，作为一种有效且持久的CO ₂还原电催化剂。基于操作X射线吸收和光电子能谱测量，具有d ⁹电子构型的单价Ni（i）原子中心被鉴定为催化活性位点。单镍原子催化剂表现出高的固有CO ₂还原活性，达到350 A g_催化剂^-1的比电流对于CO转化而言，在0.61 V的轻度过电势下，转换频率为14,800 h ^-1，法拉第效率为97％。在高达22 mA cm ^-2的CO形成电流密度下连续反应100小时后，催化剂保持其初始活性的98％。