Selective conversion of CO into ethanol on Cu(511) surface reconstructed from Cu(pc): Operando studies by electrochemical scanning tunneling microscopy, mass spectrometry, quartz crystal nanobalance, and infrared spectroscopy
- California Institute of Technology (CalTech), Pasadena, CA (United States)
- California Institute of Technology (CalTech), Pasadena, CA (United States); Univ. of California, Irvine, CA (United States)
- Univ. of California, Irvine, CA (United States)
A polycrystalline copper, surface-terminated by a well-defined (511)-oriented facet, was electrochemically generated by a series of step-wise surface reconstruction and iterations of mild oxidative-reductive processes in 0.1 M KOH. The electrochemical reduction of CO on the resultant stepped surface was investigated by four surface-sensitive operando methodologies: electrochemical scanning tunneling microscopy (STM), electrochemical quartz crystal nanobalance (EQCN), differential electrochemical mass spectrometry (DEMS), and polarization-modulation infrared spectroscopy (PMIRS). The stepped surface catalyzed the facile conversion of CO into ethanol, the exclusive alcohol product at a low overpotential of -1.06 V (SHE) or -0.3 V (RHE). The chemisorption of CO was found to be a necessary prelude to ethanol production; i.e. the surface coverages, rather than solution concentrations, of CO and its surface-bound intermediates primarily dictate the reaction rates (current densities). Contrary to the expected predominance of undercoordinated step-site reactivity over the coordination chemistry of vicinal surfaces, vibrational spectroscopic evidence reveals the involvement of terrace-bound CO adsorbates during the multi-atomic transformations associated with the production of ethanol.
- Research Organization:
- California Institute of Technology (CalTech), Pasadena, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC)
- Grant/Contract Number:
- SC0004993
- OSTI ID:
- 1801623
- Alternate ID(s):
- OSTI ID: 1598366
- Journal Information:
- Journal of Electroanalytical Chemistry, Vol. 857, Issue C; ISSN 1572-6657
- Publisher:
- ElsevierCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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