Theoretical study of transition metals supported on g-C3N4 as electrochemical catalysts for CO2 reduction to CH3OH and CH4. Issue 36 (February 2020)

• Record Type: Journal Article
• Authors: Ao, Chengcheng; Feng, Beibei; Qian, Siyu; Wang, Lei; Zhao, Wei; Zhai, Yitong; Zhang, Lidong
• Is Part Of: Journal of CO₂ utilization. Issue 36(2020)
• Page Start: 116
• Page End: 123
• Publication Date: 2020-02
• Subjects: Electrochemical CO2 reduction -- Transition metals supported on g-C3N4 -- DFT calculations; Carbon dioxide -- Periodicals; Carbon dioxide -- Environmental aspects -- Periodicals; Carbon dioxide mitigation -- Periodicals; Carbon dioxide; Carbon dioxide -- Environmental aspects; Carbon dioxide mitigation; Periodicals; 628.53205
• DOI: 10.1016/j.jcou.2019.11.007
• Languages: English
• ISSNs: 2212-9820

Abstract

Highlights: Detailed mechanisms of Fe/g-C3 N4, Co/g-C3 N4 and Ni/g-C3 N4 as catalysts applied in electrochemical CO2 reduction were investigated. Fe/g-C3 N4 exhibits excellent catalytic activity for CO2 reduction. Ni/g-C3 N4 prefers to produce CH3 OH with the limiting potential of 0.72 V. G-C3 N4 shows great potential as the platform to support transition metal for CO2 reduction system. Abstract: Electrochemical CO2 reduction has become a promising technology to address the globally accelerating CO2 emissions and produce value-add chemicals and liquid fuels. In this work, transition metals supported on graphitic carbon nitride (M/g-C3 N4, M = Fe, Co, Ni) as catalysts applied in electrochemical CO2 reduction to CH3 OH and CH4 is investigated by density functional theory (DFT) calculations. From Ni/g-C3 N4, Fe/g-C3 N4 to Co/g-C3 N4, the interaction between CO2 and catalysts is found to be gradually enhanced, especially for the adsorption of CO2 on Co/g-C3 N4, which is a typical chemical interaction. Fe/g-C3 N4 and Co/g-C3 N4 prefer to produce CH4 with limiting potentials of 0.67 V and 0.81 V, while Ni/g-C3 N4 tends to produce CH3 OH. Moreover, the electrolyte environment has little influence on the limiting potential of Fe/g-C3 N4 and Ni/g-C3 N4 . Given the superior performance of M/g-C3 N4, g-C3 N4 shows great potential as the platform to support transition metal for CO2 reduction system. These insights can be used to guide the synthesis of highly active CO2 reduction catalysts from nonprecious metals.