Lanthanide metals have attracted particular interest in the catalysis of electrochemical CO reduction. The synthesis and precise spatial distribution of active sites are fundamental important but still formidably challenging owing to the strong oxygen affinity of lanthanide. Here, heteronuclear Pr-Ni single atoms are supported on the carbon matrix containing surface framework defects from lanthanide contraction. The Pr/Ni-NC catalyst exhibits a CO Faradaic efficiency of 99.1 % with a commercial-scale current density of 237 mA cm and a turnover frequency as high as 18,038 h at −1.1 V due to d-f coupling effect and electronic structure perturbation of Pr. Furthermore, mechanistic investigations unveil that the diatomic active sites effectively reduce the energy barrier of the crucial *COOH formation, in which the Pr site facilitates CO activation and the Ni site enables HO dissociation to accelerate the proton transfer process, thereby ensuring the synergy of catalytic sites to greatly facilitate CO-to-CO conversion.

中文翻译：

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具有 Pr-N4C2 和 Ni-N4 部分的异双金属镨镍活性位点能够协同催化 CO2 电还原

镧系金属在电化学 CO 还原催化中引起了特别的兴趣。活性位点的合成和精确的空间分布至关重要，但由于镧系元素的强氧亲和力，仍然具有巨大的挑战性。在这里，异核 Pr-Ni 单原子被支撑在含有来自镧系元素收缩的表面骨架缺陷的碳基体上。 Pr/Ni-NC催化剂的CO法拉第效率为99.1%，商业规模的电流密度为237 mA cm，由于df耦合效应和Pr的电子结构扰动，在-1.1 V下的周转频率高达18,038 h。 。此外，机理研究表明，双原子活性位点有效降低了关键*COOH形成的能垒，其中Pr位点促进CO活化，Ni位点使H2O解离加速质子转移过程，从而确保催化的协同作用大大促进 CO 到 CO 的转化。