Citation: Fangfang Chang, Panpan Su, Utsab Guharoy, Runping Ye, Yanfu Ma, Huajun Zheng, Yi Jia, Jian Liu. Edge-enriched N, S co-doped hierarchical porous carbon for oxygen reduction reaction[J]. Chinese Chemical Letters, ;2023, 34(2): 107462. doi: 10.1016/j.cclet.2022.04.060 shu

Edge-enriched N, S co-doped hierarchical porous carbon for oxygen reduction reaction

Fangfang Chang ^{a, b} ,
Panpan Su ^a ,
Utsab Guharoy ^a ,
Runping Ye ^a ,
Yanfu Ma ^a ,
Huajun Zheng ^c ,
Yi Jia ^{c, *,} ,
Jian Liu ^{a, d, **,}

a.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
b.
University of Chinese Academy of Sciences, Beijing 100049, China
c.
Department of Applied Chemistry and Zhejiang Carbon Neutral Innovation Institute, Zhejiang University of Technology, Hangzhou 310032, China
d.
DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, University of Surrey, Guildford, Surrey GU2 7XH, United Kingdom

^**

jiayi@zjut.edu.cn

jian.liu@surrey.ac.uk

jianliu@dicp.ac.cn

Received Date: 26 November 2021
Revised Date: 16 March 2022
Accepted Date: 24 April 2022
Available Online: 28 April 2022

Figures(4)

The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However, the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea (TU) encapsulated in zeolitic imidazolate frameworks (TU@ZIF) composites, which delivered very good oxygen reduction reaction (ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode (RHE), good stability and methanol tolerance. Density functional theory (DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O₂ adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts.
- Porosity engineering,
- N, S co-doped carbon materials,
- Hierarchical porous carbon,
- Edge-enriched carbon,
- Oxygen reduction reaction,
- DFT calculation
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