Nitrogen-carbon materials base on pyrolytic graphene hydrogel for oxygen reduction

Guangyu Lei; Jingwen Ma; Mengyao Zhao; Shun Wu; Hongwei He; Hui Qi; Wenchao Peng; Xiaobin Fan; Guoliang Zhang; Fengbao Zhang; Yang Li

doi:10.1016/j.jcis.2021.06.036

Nitrogen-carbon materials base on pyrolytic graphene hydrogel for oxygen reduction

J Colloid Interface Sci. 2021 Nov 15:602:274-281. doi: 10.1016/j.jcis.2021.06.036. Epub 2021 Jun 8.

Authors

Guangyu Lei¹, Jingwen Ma², Mengyao Zhao³, Shun Wu⁴, Hongwei He⁵, Hui Qi⁶, Wenchao Peng⁷, Xiaobin Fan⁸, Guoliang Zhang⁹, Fengbao Zhang¹⁰, Yang Li¹¹

Affiliations

¹ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China. Electronic address: guangyulei@tju.edu.cn.
² State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China. Electronic address: jingwenma@cup.edu.cn.
³ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China. Electronic address: Zhaomy@tju.edu.cn.
⁴ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China. Electronic address: wushun1895@tju.edu.cn.
⁵ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China. Electronic address: hehongwei@tju.edu.cn.
⁶ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China. Electronic address: qihui1101@tju.edu.cn.
⁷ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China; Chemistry and Chemical Engineering Guangdong Laboratory, Shantou 515031 China. Electronic address: wenchao.peng@tju.edu.cn.
⁸ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China; Chemistry and Chemical Engineering Guangdong Laboratory, Shantou 515031 China. Electronic address: xiaobinfan@tju.edu.cn.
⁹ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China. Electronic address: zhangguoliang@tju.edu.cn.
¹⁰ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China. Electronic address: fbzhang@tju.edu.cn.
¹¹ Lab of Advanced Nano-structures & Transfer Processes, Department of Chemical Engineering, Tianjin University, Tianjin 300354, China; Chemistry and Chemical Engineering Guangdong Laboratory, Shantou 515031 China. Electronic address: liyang1895@tju.edu.cn.

PMID: 34130174
DOI: 10.1016/j.jcis.2021.06.036

Abstract

Hypothesis: Oxygen reduction reaction (ORR) has played a significant role in the utilization of energy nowadays. Nitrogen-doped carbon materials are seen as promising catalysts for ORR, so it is of great significance in studying the functions of different nitrogen moieties.

Experiments: The graphene hydrogel-based nitrogen-arbon materials (GH N-C) were fabricated by first obtaining a gel through hydrothermal treatment using graphene oxide (GO) as precursor, and then calcined in an ammonia atmosphere at different temperatures to form N-doped graphitized materials with divers nitrogen configuration.

Findings: GH N-C materials with tunable nitrogen configuration were synthesized by a two-step method base on graphene hydrogel. Benefiting from the 3D hydrogel structure, rich defects and optimized chemical properties, GH N-C-900 prepared by NH₃ pyrolysis at 900 °C exhibits an excellent electrocatalytic performance toward ORR, with the onset potential of 0.947 ± 0.013 V versus RHE, half-wave potential of 0.830 ± 0.010 V versus RHE, electron transfer number of 3.61-3.99, along as methanol tolerance and superior long-term stability. Comprehensive studies have shown that there is a positive correlation between the total amount of pyrrolic-N and quaternary-N and the catalytic performance of ORR.

Keywords: Fuel cell; Graphene; Hydrogel; Nitrogen configuration; Oxygen reduction reaction.