1. Nitrogen and sulfur dual-doped high-surface-area hollow carbon nanospheres for efficient CO2 reduction
- Author
-
Yu Wu, Yongjie Qin, Qi Hu, Jianhong Liu, Chuanxin He, Lei Pei, Qianling Zhang, Hengpan Yang, and Guodong Li
- Subjects
Materials science ,chemistry.chemical_element ,02 engineering and technology ,General Medicine ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Electrochemistry ,01 natural sciences ,0104 chemical sciences ,Gibbs free energy ,Catalysis ,symbols.namesake ,chemistry ,Chemical engineering ,Specific surface area ,symbols ,0210 nano-technology ,Selectivity ,Pyrolysis ,Carbon ,Faraday efficiency - Abstract
The electrochemical reduction of CO2 (CO2RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials (SZ-HCN) as CO2RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area (1510 m2 g−g1) exhibited efficient electrocatalytic activity and selectivity for CO2RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency (~93%) at −0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2RR activity.
- Published
- 2020