Boosting electrochemical CO2 reduction on ternary heteroatoms-doped porous carbon

Fangqi Yang, Haoming Yu, Xinyu Mao, Qiangguo Meng, Shixia Chen, Qiang Deng, Zheling Zeng, Jun Wang, Shuguang Deng

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Electroreduction of CO2 to value-added chemicals using metal-free carbon catalysts is attractive, but single N-doped carbons suffer from poor efficiency (<90%) and low current density (<2 mA cm−2). Herein, we report a facile and scalable preparation of ternary heteroatoms (N, S, P)-doped carbon electrocatalyst to enhance electrochemical activity, because the multi-heteroatoms with different sizes and electronegativities can modulate the electronic properties to facilitate CO2 localization and provide abundant active sites with enhanced charge-carrier concentrations. It exhibits high activity toward CO2 electroreduction to CO activity with 92% CO Faradaic efficiency (FECO) at −0.7 VRHE and low onset overpotential of 270 mV. The promising potential of industrial application is manifested by the high current density of 245 mA cm−2 and stable FECO above 98% in a flow-cell configuration. Moreover, in-situ Raman spectroscopy demonstrates that *COOH is the key intermediate in CO2-to-CO conversion. Density functional theory calculations reveal that the synergistic effect of N, S, and P heteroatoms boosts the catalytic activity by greatly decreasing the free energy barrier of *COOH formation. Furthermore, the morphological benefit of hierarchically porous structures plays a synergistic role in improving the CO2 reduction activity.

Original languageEnglish (US)
Article number131661
JournalChemical Engineering Journal
Volume425
DOIs
StatePublished - Dec 1 2021

Keywords

  • CO reduction
  • Electrocatalysis
  • Porous carbon
  • Synergistic effect
  • Ternary-doping

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Chemical Engineering(all)
  • Industrial and Manufacturing Engineering

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