Electrochemical CO2 Reduction to C1 Products on Single Nickel/Cobalt/Iron‐Doped Graphitic Carbon Nitride: A DFT Study

• DOI: 10.1002/cssc.201902483
• Publication Date: 2019-10-10T20:01:56Z
• Authors: Chen Guo; Tian Zhang; Xiangxuan Deng; Xiongyi Liang; Wenyue Guo; Xiaoqing Lu; Chi‐Man Lawrence Wu
• Keywords: Carbon fibers; Graphitic carbon nitride

Electrocatalytic CO2 reduction reaction (CRR) is one of the most promising strategies to convert greenhouse gases energy sources. Herein, CRR was applied towards making C1 products (CO, HCOOH, CH3 OH, and CH4 ) on g-C3 N4 frameworks with single Ni, Co, Fe introduction; this process investigated by density functional theory. The structures electrocatalysts, adsorption configurations, mechanisms were systematically studied. Results showed that located from corner cavity center. Analyses configurations electronic suggested could be chemically adsorbed Co-C3 Fe-C3 , but physically Ni-C3 . H2 evolution (HER), as a suppression CRR, investigated, results exhibited more selectivity than HER. proceeded via COOH OCHO initial protonation intermediates Co/Fe-C3 respectively, which resulted in different along quite pathways. Compared had favorable activity for OH production unique rate-limiting steps lower limiting potential.