New reaction path for long-chain hydrocarbons by electrochemical CO2 and CO reduction over Au/stainless steel

Chemosphere. 2023 Oct:338:139616. doi: 10.1016/j.chemosphere.2023.139616. Epub 2023 Jul 21.

Abstract

The Fischer-Tropsch (F-T) synthesis is recognized for its ability to produce long-chain hydrocarbons. In this study, we aimed to replicate F-T synthesis using electrochemical CO2 reduction and CO reduction reactions on a stainless steel (SS) support with a gold (Au) overlayer. Under CO2-saturated conditions, the presence of Au on the SS surface led to the formation of CH4 and a range of hydrocarbons (CnH2n and CnH2n+2, n = 2-7), while bare SS primarily produced hydrogen. The Au(10 nm)/SS exhibited the highest hydrocarbon production in CO2-saturated phosphate, indicating a synergistic effect at the Au-SS interface. In CO-saturated conditions, bare SS also produced long-chain hydrocarbons, but increasing Au thickness resulted in decreased production due to poor CO adsorption. Hydrocarbons were formed through both direct and indirect CO adsorption pathways. Anderson-Schulz-Flory analysis confirmed surface CO hydrogenation and C-C coupling polymerization following conventional F-T synthesis. The C2 hydrocarbons exhibited distinct behavior compared to C3-5 hydrocarbons, suggesting different reaction pathways. Despite low reduction product levels, our EC method successfully replicated F-T synthesis using the Au/SS electrode, providing valuable insights into C-C coupling mechanisms and electrochemical production of long-chain hydrocarbons. Depth-profiling X-ray photoelectron spectroscopy revealed significant changes in surface elemental compositions before and after EC reduction.

Keywords: Au/stainless steel; Depth-profiling X-ray photoelectron spectroscopy; Electrochemical CO reduction; Electrochemical CO(2) reduction; Fischer–Tropsch synthesis.

MeSH terms

  • Carbon Dioxide* / chemistry
  • Hydrocarbons
  • Hydrogen / chemistry
  • Hydrogenation
  • Stainless Steel* / chemistry

Substances

  • Stainless Steel
  • Carbon Dioxide
  • Hydrocarbons
  • Hydrogen