Lan Yangchun, Niu Gaoqiang, Wang Fei, Cui Dehu, Hu Zhuofeng
School of Microelectronics, Southern University of Science and Technology, Shenzhen 518055, P. R. China.
School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou 510275, P. R. China.
ACS Appl Mater Interfaces. 2020 Aug 12;12(32):36128-36136. doi: 10.1021/acsami.0c09240. Epub 2020 Aug 4.
Electrochemical reduction of CO was a widespread method for CO conversion into valuable chemical fuel. CH is an important product from CO reduction. However, conversion of CO into the hydrocarbon CH faced large energy barriers. Herein, we, for the first time, achieve a high efficiency for electrochemical conversion of CO to CH on a tin-modified CuO. By modifying with Sn, we obtained a related low onset potential of CH as positive as -0.8 V RHE and a high Faradaic efficiency of CH as high as 22% at -1.0 V ( RHE). According to density functional calculation, the Sn dopant mainly enriched the electron density of CuO, while it was electron-poor in the Sn dopants. The rate of CO reduction can be enhanced on Cu nanosheets with higher electron density. We believed that this work would promote the development of two-dimensional catalysts for CO conversion and deepen the understanding of doping on CO reduction.
电化学还原CO是将CO转化为有价值化学燃料的一种广泛应用的方法。CH是CO还原的重要产物。然而，将CO转化为碳氢化合物CH面临着较大的能量障碍。在此，我们首次在锡修饰的CuO上实现了将CO高效电化学转化为CH。通过用Sn进行修饰，我们获得了CH相关的低起始电位，正向高达 -0.8 V（相对于可逆氢电极，RHE），并且在 -1.0 V（RHE）时CH的法拉第效率高达22%。根据密度泛函计算，Sn掺杂剂主要富集了CuO的电子密度，而Sn掺杂剂中电子匮乏。在具有较高电子密度的Cu纳米片上可以提高CO还原速率。我们相信这项工作将推动用于CO转化的二维催化剂的发展，并加深对掺杂促进CO还原的理解。
