Chen Peng, Zhang Pei, Kang Xinchen, Zheng Lirong, Mo Guang, Wu Ruizhi, Tai Jing, Han Buxing
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190 China.
School of Chemistry, University of Chinese Academy of Sciences, Beijing 100049 China.
J Am Chem Soc. 2022 Aug 17;144(32):14769-14777. doi: 10.1021/jacs.2c05373. Epub 2022 Aug 4.
Non-copper electrocatalysts are seldom reported to generate C products, and the efficiency over these catalysts is low. In this work, we report a nitrogen-doped γ-FeO (FeO-N@CN) electrocatalyst, which yield CH as the major product in an H-cell. At -2.0 V vs Ag/Ag, the Faradaic efficiency (FE) for ethane reaches 42% with a current density of 32 mA cm. This is the first report about selective CO reduction to ethane (CH) over an iron-based catalyst. The results showed that the catalyst possessing FeON sites enriched with oxygen vacancies was beneficial for the stabilization of *COOH intermediates. The exposure of two adjacent surfaces of Fe atoms was conducive to lowering the energy barrier for C-C coupling over FeON sites, facilitating the generation of CH. This work provides a strategy for the design of a novel iron-based catalyst with tunable local coordination and electronic structures for converting CO into C products in the CORR.
很少有报道称非铜电催化剂能生成C产物，且这些催化剂的效率较低。在这项工作中，我们报道了一种氮掺杂的γ-FeO（FeO-N@CN）电催化剂，它在H型电解池中以CH作为主要产物。在相对于Ag/Ag为-2.0 V时，乙烷的法拉第效率（FE）达到42%，电流密度为32 mA cm。这是关于在铁基催化剂上选择性将CO还原为乙烷（CH）的首次报道。结果表明，具有富含氧空位的FeON位点的催化剂有利于*COOH中间体的稳定。两个相邻Fe原子表面的暴露有利于降低FeON位点上C-C偶联的能垒，促进CH的生成。这项工作为设计一种具有可调局部配位和电子结构的新型铁基催化剂提供了策略，用于在CO还原反应中将CO转化为C产物。
