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Switching CO2 electroreduction selectivity between CO and HCOOH on poly(ionic liquid)-Ag hybrids.

Ang Li1, Guo-Yi Duan2, Yue Pan2

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Researchers engineered poly(ionic liquid)-silver (PIL-Ag) hybrids to control the electrocatalytic conversion of CO2. Alkyl chain length tuned silver sites, enabling selective switching between CO and HCOOH production for efficient energy conversion.

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Area of Science:

  • Electrocatalysis
  • Materials Science
  • Green Chemistry

Background:

  • Electrocatalytic conversion of carbon dioxide (CO2) to carbon monoxide (CO) and formic acid (HCOOH) is a promising route for energy-efficient chemical synthesis.
  • Achieving high selectivity and efficiency in CO2 electroreduction reaction (CO2RR) remains a significant challenge, particularly in controlling product distribution.
  • Silver (Ag) based electrocatalysts show potential for CO2RR, but tuning their activity and selectivity requires precise control over active sites and reaction conditions.

Purpose of the Study:

  • To develop poly(ionic liquid)-silver (PIL-Ag) hybrid materials for tunable electrocatalytic CO2 conversion.
  • To investigate the influence of alkyl chain length in PIL-Ag hybrids on the selectivity between CO and HCOOH production.
  • To elucidate the mechanistic pathways governing the formation of *COOH and *H intermediates and their role in product selectivity.

Main Methods:

  • Fabrication of poly(ionic liquid)-silver (PIL-Ag) hybrids with varying alkyl chain lengths.
  • Electrochemical characterization of PIL-Ag hybrids using techniques such as cyclic voltammetry and chronoamperometry.
  • Operando mechanistic studies to analyze intermediate formation (*COOH, *H) and mass transfer effects of CO2 and H2O.
  • Evaluation of Faradaic efficiency (FE) for CO and HCOOH production at different current densities.

Main Results:

  • Alkyl chain length in PIL-Ag hybrids significantly influenced the structure and intrinsic activity of Ag sites, affecting CO2RR selectivity.
  • Ag@PIL-C(4)-0.5 exhibited a high HCOOH to CO Faradaic efficiency ratio (FEHCOOH/FECO = 1.45), while Ag@PIL-C(6)-0.5 favored CO production.
  • Optimized conditions on Ag@PIL-C(6)-2.0 demonstrated a significant increase in FEHCOOH/FECO ratio (0.87) with low H2 evolution (<5.0%) by increasing current density.

Conclusions:

  • PIL-Ag hybrids offer a versatile platform for tuning the selectivity of CO2 electrocatalytic conversion by controlling Ag active site properties and mass transport.
  • The enrichment of *H intermediates relative to *CO2 intermediates at Ag sites is crucial for promoting *OCHO formation and enhancing HCOOH selectivity.
  • This study provides insights into designing advanced electrocatalysts for efficient and selective CO2 conversion into valuable chemical feedstocks.