Electrochemical Reduction of Carbon Dioxide at Gold-Palladium Core–Shell Nanoparticles: Product Distribution versus Shell Thickness

Jo L Humphrey, Daniela Plana, Veronica Celorrio, Sajanikumari Sadasivan, Robert Tooze, Paramaconi Rodriguez, David J Fermin

Research output: Contribution to journalArticle (Academic Journal)peer-review

39 Citations (Scopus)
273 Downloads (Pure)

Abstract

The electrocatalytic reduction of CO2 at carbon-supported Au-Pd core–shell nanoparticles is investigated systematically as a function of the Pd shell thickness. Liquid- and gas-phase products were determined by off-line 1H NMR spectroscopy and on-line electrochemical mass spectrometry. Our results uncover the relationship between the nature of the products generated and the Pd shell thickness. CO and H2 are the only products generated at 1 nm thick shells, whereas shells of 5 and 10 nm produced HCOO, CH4 and C2H6. The concentration of HCOO detected in the electrolyte was dependent on the applied potential and reached a maximum Faradaic efficiency of 27 % at −0.5 V versus the reversible hydrogen electrode for 10 nm thick shells. We conclude that collisions between absorbed hydrogen at relaxed Pd lattices and strongly bound “CO-like” intermediates promote the complete hydrogenation to C1 and C2 alkanes without the generation of other products, such as alcohols and aldehydes.
Original languageEnglish
Pages (from-to)952-960
Number of pages9
JournalChemCatChem
Volume8
Issue number5
Early online date8 Jan 2016
DOIs
Publication statusPublished - 1 Mar 2016

Keywords

  • Carbon Dioxide
  • Electrocatalysis
  • Hydrogenation
  • Palladium
  • Structure-Activity Relationships

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