4.7 Article

Triple-phase electrocatalysis for the enhanced CO2 reduction to HCOOH on a hydrophobic surface

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 405, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2020.126975

Keywords

Electrochemical CO2 reduction reaction; Wettability; HCOOH; Cu/Sn electrode; Triple-phase interface

Funding

  1. National Natural and Science Foundation of China [51776025]
  2. Natural Science Funds for Distinguished Young Scholar of Chongqing [cstc2019jcyjjqX0020]
  3. Fundamental Research Funds for the Central Universities [2018CDPTCG0001/18]

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Introducing a hydrophobic surface on Cu/Sn nanowires can significantly improve the Faraday efficiency for HCOOH production and achieve excellent CO2 conversion activity even at high overpotential. The rich triple-phase interfaces at the hydrophobic surface enhance CO2 mass transfer and increase the selectivity of HCOOH, providing a facile and promising approach for improved electrochemical CO2 reduction.
The aqueous electrochemical reduction of CO2 into hydrocarbon fuels has been considered as a promising route to mitigate environmental problems. However, owing to the limited mass transfer of CO2 and competition with hydrogen evolution reaction in aqueous electrolyte solution, Sn-based catalysts exhibited low current density and low Faraday efficiency (FE), especially at high overpotential. Herein, we introduced a hydrophobic surface on Cu/Sn nanowires by decoration with trimethoxy (1H, 1H, 2H, 2H-heptadecafluorodecyl) silane (FAS). In contrast to the hydrophilic electrode (FEHCOOH-76.44%, at - 1.2 V vs. RHE), the hydrophobic electrode achieved a high Faraday efficiency of 94.17% towards HCOOH production at -1.2 V vs. RHE. Remarkably, the synthesized electrode achieved an excellent activity for CO2 conversion even at high overpotential (FEHCOOH-86.39%, j(HCOOH)-23.95 mA cm(-2) , at -1.4 V vs. RHE), which far exceeded other most of Sn materials. This observation could be contributed to the rich triple-phase interfaces at the hydrophobic surface, which enhanced the CO2 mass transfer and increased the selectivity of HCOOH, especially at high overpotential. It was demonstrated that increasing CO2 mass transfer flux through the reduction of the wettability of the electrode was a facile and promising approach for the improved electrochemical CO(2 )reduction.

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