Hu Weibo, Li Jiejie, Ma Lushan, Su Wanyu, Zhu Yanping, Li Wenhao, Chen Yubin, Zou Liangliang, Zou Zhiqing, Yang Bo, Wen Ke, Yang Hui
Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China.
University of Chinese Academy of Sciences, Beijing 100039, China.
ACS Appl Mater Interfaces. 2021 Dec 8;13(48):57462-57469. doi: 10.1021/acsami.1c18902. Epub 2021 Nov 29.
Although great progress has been made in the field of electrochemical CO reduction reaction (eCORR), inducing product selectivity is still difficult. We herein report that a thiocyanate ion (SCN) switched the product selectivity of copper catalysts for eCORR in an H-cell. A cuprous thiocyanate-derived Cu catalyst was found to exhibit excellent HCOOH selectivity (faradaic efficiency = 70-88%) over a wide potential range (-0.66 to -0.95 V vs RHE). Furthermore, it was revealed that the formation of CO and CH over commercial copper electrodes could be dramatically suppressed with the presence of SCN, switching to HCOOH. Density functional theory calculations disclosed that SCN made the formation of HCOO* easier than COOH* on Cu (211), facilitating the HCOOH generation. Our results provide a new insight into eCORR and will be helpful in the development of cheap electrocatalysts for specific utilization.
尽管电化学CO还原反应（eCORR）领域已取得巨大进展，但诱导产物选择性仍然困难。我们在此报告，硫氰酸根离子（SCN）在H型电池中改变了用于eCORR的铜催化剂的产物选择性。发现一种由硫氰酸亚铜衍生的Cu催化剂在很宽的电位范围内（相对于可逆氢电极，-0.66至-0.95 V）表现出优异的HCOOH选择性（法拉第效率=70-88%）。此外，研究表明，在SCN存在下，商业铜电极上CO和CH的形成可被显著抑制，转而生成HCOOH。密度泛函理论计算表明，SCN使Cu（211）上HCOO的形成比COOH更容易，促进了HCOOH的生成。我们的结果为eCORR提供了新的见解，并将有助于开发用于特定用途的廉价电催化剂。
