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 () and Yanglong Hou ()
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Kesong Tian: Yanshan University
Junyan Wang: Yanshan University
Ling Cao: Yanshan University
Wei Yang: Yanshan University
Wanchun Guo: Yanshan University
Shuhu Liu: Chinese Academy of Sciences
Wei Li: Peking University
Fengyan Wang: Yanshan University
Xueai Li: Yanshan University
Zhaopeng Xu: Yanshan University
Zhenbo Wang: Harbin Institute of Technology
Haiyan Wang: Yanshan University
Yanglong Hou: Peking University

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-17727-y

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