Tan Yucan, Niu Yueheng, Ji Xu, Cui Xiuhua, Duan Haiming, Jing Qun
Xinjiang Key Laboratory of Solid State Physics and Devices, School of Physical Science and Technology, Xinjiang University, Urumqi 830017, China.
Langmuir. 2025 Mar 25;41(11):7912-7921. doi: 10.1021/acs.langmuir.5c00728. Epub 2025 Mar 11.
Single-atom catalysts (SACs) have displayed unprecedented activity and selectivity for electrochemical CO reduction reaction (CORR). Herein, a series of metal single atoms embedded on nitrogen-doped graphene (M-NG, where M = In, Tl, Ge, Sn, Pb, Sb, and Bi) is systematically evaluated as CORR electrocatalysts by density functional theory (DFT) calculations. The computational results show that most M-NG exhibit better CORR selectivity over the hydrogen evolution reaction (HER). Ge/Pb-NG exhibits excellent electrocatalytic performance in the generation of HCOOH from the CORR with low limiting potentials of -0.292 and -0.306 V, which surpass the performance of the vast majority of electrocatalysts. Adsorption energy of the key intermediate *HCOO can be used as an effective reactivity reaction descriptor to screen promising CORR catalysts. The results of this work highlight M-NG as an ideal electrochemical for the electrocatalytic CORR.
单原子催化剂（SACs）在电化学CO还原反应（CORR）中展现出了前所未有的活性和选择性。在此，通过密度泛函理论（DFT）计算，系统评估了一系列嵌入氮掺杂石墨烯的金属单原子（M-NG，其中M = In、Tl、Ge、Sn、Pb、Sb和Bi）作为CORR电催化剂的性能。计算结果表明，大多数M-NG在析氢反应（HER）方面表现出比CORR更好的选择性。Ge/Pb-NG在CORR生成HCOOH的过程中展现出优异的电催化性能，其低极限电位分别为-0.292和-0.306 V，超过了绝大多数电催化剂的性能。关键中间体*HCOO的吸附能可作为筛选有前景的CORR催化剂的有效反应活性描述符。这项工作的结果突出了M-NG作为CORR电催化的理想电化学材料。
