Citation: Guodong Li, Yongjie Qin, Yu Wu, Lei Pei, Qi Hu, Hengpan Yang, Qianling Zhang, Jianhong Liu, Chuanxin He. Nitrogen and sulfur dual-doped high-surface-area hollow carbon nanospheres for efficient CO₂ reduction[J]. Chinese Journal of Catalysis, ;2020, 41(5): 830-838. doi: S1872-2067(19)63485-6 shu

Nitrogen and sulfur dual-doped high-surface-area hollow carbon nanospheres for efficient CO₂ reduction

Guodong Li ^a,b, ,
Yongjie Qin ^b ,
Yu Wu ^a,b ,
Lei Pei ^b ,
Qi Hu ^b ,
Hengpan Yang ^b ,
Qianling Zhang ^b ,
Jianhong Liu ^b ,
Chuanxin He ^b

a Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, Anhui, China;
b Shenzhen Key Laboratory for Functional Polymer, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, Guangdong, China

Received Date: 25 September 2019
Revised Date: 29 October 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (21574084, 21571131), the Natural Science Foundation of Guangdong (2017A040405066), and Shenzhen Government's Plan of Science and Technology (JCYJ20160308104704791, JCYJ20170818091657056).

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^-1) 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.
- High specific surface area,
- Hollow structure,
- Carbon-based catalysts,
- CO₂ reduction reaction,
- Electrocatalytic selectivity
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Nitrogen and sulfur dual-doped high-surface-area hollow carbon nanospheres for efficient CO₂ reduction