Journal
CHEMCATCHEM
Volume 8, Issue 5, Pages 952-960Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201501260
Keywords
electrochemistry; gold; hydrogenation; palladium; structure-activity relationships
Categories
Funding
- Sasol Technology (UK) Ltd.
- NERC
- Royal Society
- UK National Academy though the Newton International Fellows program
- EPSRC [EP/K007025/1, EP/K035746/1, EP/M028216/1]
- University of Birmingham through the Birmingham fellowship program
- UoB
- Engineering and Physical Sciences Research Council [EP/K007025/1, EP/K035746/1, EP/M028216/1, EP/L022532/1] Funding Source: researchfish
- Natural Environment Research Council [1237945] Funding Source: researchfish
- EPSRC [EP/K035746/1, EP/L022532/1, EP/K007025/1, EP/M028216/1, EP/K014706/2] Funding Source: UKRI
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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 (HNMR)-H-1 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 H-2 are the only products generated at 1nm thick shells, whereas shells of 5 and 10nm 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 -0.5V versus the reversible hydrogen electrode for 10nm 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.
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