Dramatic HER Suppression on Ag Electrodes via Molecular Films for Highly Selective CO2 to CO Reduction

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2021
Autor:innen
Rosas-Hernández, Alonso
Fontani Herreros, Alex M.
Agapie, Theodor
Peters, Jonas C.
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European Union (EU): 793471
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COOLEFIN: Novel Dinuclear Late Transition Metal Catalysts for CO2/Olefin and CO2/Epoxide/olefin Copolymerization
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ACS Catalysis. ACS Publications. 2021, 11(8), pp. 4530-4537. eISSN 2155-5435. Available under: doi: 10.1021/acscatal.1c00338
Zusammenfassung

The carbon dioxide reduction reaction (CO2RR) in aqueous electrolytes suffers from efficiency loss due to the competitive hydrogen evolution reaction (HER). Developing efficient methods to suppress HER is a crucial step toward CO2 utilization. Herein we report the selective conversion of CO2 to CO on planar silver electrodes with Faradaic efficiencies >99% using simple pyridinium-based additives. Similar to our previous studies on copper electrodes, the additives form an organic film which alters CO2RR selectivity. We report electrochemical kinetic and other mechanistic data to shed light on the role of these organic layers in suppressing HER. These data suggest that hydrogen production is selectively inhibited by the growth of a hydrophobic organic layer on the silver surface that limits proton but not CO2 mass transport at certain applied potentials. The data also point to the involvement of a proton-transfer within the rate-determining step of the catalysis, instead of the commonly observed electron-transfer step for the case of planar Ag electrodes.

Zusammenfassung in einer weiteren Sprache
Fachgebiet (DDC)
540 Chemie
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electrocatalysis, CO2RR, HER, solar fuels, modified electrodes, silver electrodes
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ISO 690THEVENON, Arnaud, Alonso ROSAS-HERNÁNDEZ, Alex M. FONTANI HERREROS, Theodor AGAPIE, Jonas C. PETERS, 2021. Dramatic HER Suppression on Ag Electrodes via Molecular Films for Highly Selective CO2 to CO Reduction. In: ACS Catalysis. ACS Publications. 2021, 11(8), pp. 4530-4537. eISSN 2155-5435. Available under: doi: 10.1021/acscatal.1c00338
BibTex
@article{Thevenon2021Drama-53684,
  year={2021},
  doi={10.1021/acscatal.1c00338},
  title={Dramatic HER Suppression on Ag Electrodes via Molecular Films for Highly Selective CO<sub>2</sub> to CO Reduction},
  number={8},
  volume={11},
  journal={ACS Catalysis},
  pages={4530--4537},
  author={Thevenon, Arnaud and Rosas-Hernández, Alonso and Fontani Herreros, Alex M. and Agapie, Theodor and Peters, Jonas C.}
}
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