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

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

180 Citations (Scopus)

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
Publication statusPublished - 19 Nov 2018
Externally publishedYes

Keywords

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

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