Boosting the Proton-coupled Electron Transfer via Fe−P Atomic Pair for Enhanced Electrochemical CO2 Reduction

Qiao Zhang, Hsin Jung Tsai, Fuhua Li, Zhiming Wei, Qinye He, Jie Ding, Yuhang Liu, Zih Yi Lin, Xiaoju Yang, Zhaoyang Chen, Fangxin Hu, Xuan Yang, Qing Tang*, Hong Bin Yang*, Sung Fu Hung*, Yueming Zhai*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

5 Scopus citations

Abstract

Single-atom catalysts exhibit superior CO2-to-CO catalytic activity, but poor kinetics of proton-coupled electron transfer (PCET) steps still limit the overall performance toward the industrial scale. Here, we constructed a Fe−P atom paired catalyst onto nitrogen doped graphitic layer (Fe1/PNG) to accelerate PCET step. Fe1/PNG delivers an industrial CO current of 1 A with FECO over 90 % at 2.5 V in a membrane-electrode assembly, overperforming the CO current of Fe1/NG by more than 300 %. We also decrypted the synergistic effects of the P atom in the Fe−P atom pair using operando techniques and density functional theory, revealing that the P atom provides additional adsorption sites for accelerating water dissociation, boosting the hydrogenation of CO2, and enhancing the activity of CO2 reduction. This atom-pair catalytic strategy can modulate multiple reactants and intermediates to break through the inherent limitations of single-atom catalysts.

Original languageEnglish
Article numbere202311550
JournalAngewandte Chemie - International Edition
Volume62
Issue number44
DOIs
StatePublished - 26 Oct 2023

Keywords

  • Electrochemical CORR
  • Proton-Coupled Electron Transfer
  • Single-Atom Catalysis
  • Water Dissociation

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