Single-site pyrrolic-nitrogen-doped sp2-hybridized carbon materials and their pseudocapacitance

Kesong Tian; Junyan Wang; Ling Cao; Wei Yang; Wanchun Guo; Shuhu Liu; Wei Li; Fengyan Wang; Xueai Li; Zhaopeng Xu; Zhenbo Wang; Haiyan Wang; Yanglong Hou

doi:10.1038/s41467-020-17727-y

Single-site pyrrolic-nitrogen-doped sp²-hybridized carbon materials and their pseudocapacitance

Nat Commun. 2020 Aug 4;11(1):3884. doi: 10.1038/s41467-020-17727-y.

Authors

Kesong Tian^{1

2

3}, Junyan Wang³, Ling Cao³, Wei Yang³, Wanchun Guo^{4

5}, Shuhu Liu⁶, Wei Li², Fengyan Wang³, Xueai Li^{1

3}, Zhaopeng Xu¹, Zhenbo Wang⁷, Haiyan Wang^{8

9}, Yanglong Hou¹⁰

Affiliations

¹ State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, 066004, Qinhuangdao, China.
² Beijing Innovation Center for Engineering Science and Advanced Technology (BIC-ESAT), College of Engineering, Peking University, 100871, Beijing, China.
³ Hebei Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering, Yanshan University, 066004, Qinhuangdao, China.
⁴ State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, 066004, Qinhuangdao, China. wc-g@ysu.edu.cn.
⁵ Hebei Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering, Yanshan University, 066004, Qinhuangdao, China. wc-g@ysu.edu.cn.
⁶ Institute of High Energy Physics, Chinese Academy of Sciences, 100049, Beijing, China.
⁷ School of Chemistry and Chemical Engineering, Harbin Institute of Technology, 150080, Harbin, China.
⁸ State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, 066004, Qinhuangdao, China. hywang@ysu.edu.cn.
⁹ Hebei Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering, Yanshan University, 066004, Qinhuangdao, China. hywang@ysu.edu.cn.
¹⁰ Beijing Innovation Center for Engineering Science and Advanced Technology (BIC-ESAT), College of Engineering, Peking University, 100871, Beijing, China. hou@pku.edu.cn.

Abstract

Integrating nitrogen species into sp²-hybridized carbon materials has proved an efficient means to improve their electrochemical performance. Nevertheless, an inevitable mixture of nitrogen species in carbon materials, due to the uncontrolled conversion among different nitrogen configurations involved in synthesizing nitrogen-doped carbon materials, largely retards the precise identification of electrochemically active nitrogen configurations for specific reactions. Here, we report the preparation of single pyrrolic N-doped carbon materials (SPNCMs) with a tunable nitrogen content from 0 to 4.22 at.% based on a strategy of low-temperature dehalogenation-induced and subsequent alkaline-activated pyrolysis of 3-halogenated phenol-3-aminophenol-formaldehyde (X-APF) co-condensed resins. Additionally, considering that the pseudocapacitance of SPNCMs is positively dependent on the pyrrolic nitrogen content, it could be inferred that pyrrolic nitrogen species are highly active pseudocapacitive sites for nitrogen-doped carbon materials. This work gives an ideal model for understanding the contribution of pyrrolic nitrogen species in N-doped carbon materials.

Abstract

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