Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 56, Issue 13, Pages 3621-3624Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201700580
Keywords
CO dimer; CO reduction; DFT calculations; electrocatalysis; IR spectroscopy
Categories
Funding
- Netherlands Organization for Scientific Research (NWO), Veni [722.014.009]
- NWO Physical Sciences
- NWO
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Carbon dioxide and carbon monoxide can be electrochemically reduced to useful products such as ethylene and ethanol on copper electrocatalysts. The process is yet to be optimized and the exact mechanism and the corresponding reaction intermediates are under debate or unknown. In particular, it has been hypothesized that the C-C bond formation proceeds via CO dimerization and further hydrogenation. Although computational support for this hypothesis exists, direct experimental evidence has been elusive. In this work, we detect a hydrogenated dimer intermediate (OCCOH) using Fourier transform infrared spectroscopy at low over-potentials in LiOH solutions. Density functional theory calculations support our assignment of the observed vibrational bands. The formation of this intermediate is structure sensitive, as it is observed only during CO reduction on Cu(100) and not on Cu(111), in agreement with previous experimental and computational observations.
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