Composition Tailoring via N and S Co-doping and Structure Tuning by Constructing Hierarchical Pores: Metal-Free Catalysts for High-Performance Electrochemical Reduction of CO2

Hengpan Yang, Yu Wu, Qing Lin, Liangdong Fan, Xiaoyan Chai, Qianling Zhang, Jianhong Liu, Chuanxin He, Zhiqun Lin

Research output: Contribution to journalArticlepeer-review

166 Scopus citations

Abstract

A facile route to scalable production of N and S co-doped, hierarchically porous carbon nanofiber (NSHCF) membranes (ca. 400 cm2 membrane in a single process) is reported. As-synthesized NSHCF membranes are flexible and free-standing, allowing their direct use as cathodes for efficient electrochemical CO2 reduction reaction (CO2RR). Notably, CO with 94 % Faradaic efficiency and −103 mA cm−2 current density are readily achieved with only about 1.2 mg catalyst loading, which are among the best results ever obtained by metal-free CO2RR catalysts. On the basis of control experiments and DFT calculations, such outstanding CO Faradaic efficiency can be attributed to the co-doped pyridinic N and carbon-bonded S atoms, which effectively decrease the Gibbs free energy of key *COOH intermediate. Furthermore, hierarchically porous structures of NSHCF membranes impart a much higher density of accessible active sites for CO2RR, leading to the ultra-high current density.

Original languageEnglish
Pages (from-to)15476-15480
Number of pages5
JournalAngewandte Chemie - International Edition
Volume57
Issue number47
DOIs
StatePublished - 19 Nov 2018

Bibliographical note

Funding Information:
The financial support of the National Natural Science Foundation (NNSF) of China (21574084 and 21571131), the Natural Science Foundation of Guangdong Province (2015A030313554 and 2017A040405066), and Shenzhen Government's Plan of Science and Technology (JCYJ20160308104704791, JCYJ20170817095041212, and JCYJ20170818091657056) are gratefully acknowledged.

Funding Information:
The financial support of the National Natural Science Foundation (NNSF) of China (21574084 and 21571131), the Natural Science Foundation of Guangdong Province (2015A030313554 and 2017A040405066), and Shenzhen Government≫s Plan of Science and Technology (JCYJ20160308104704791, JCYJ20170817095041212, and JCYJ20170818091657056) are gratefully acknowledged.

Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

  • CO reduction
  • electrocatalysis
  • hierarchical pores
  • metal-free catalysts
  • ultrahigh current density

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