Reprint of "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"

Baricuatro, Jack H.; Kim, Youn-Geun; Tsang, Chu F.; Javier, Alnald C.; Cummins, Kyle D.; Hemminger, John C.

doi:10.1016/j.jelechem.2020.114757

Reprint of "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"

Journal Article · Tue Oct 13 00:00:00 EDT 2020 · Journal of Electroanalytical Chemistry

DOI:https://doi.org/10.1016/j.jelechem.2020.114757· OSTI ID:1850862

Baricuatro, Jack H. ^[1]; ^[2]; Tsang, Chu F. ^[3]; Javier, Alnald C. ^[2]; Cummins, Kyle D. ^[2]; Hemminger, John C. ^[4]

California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis. Division of Chemistry and Chemical Engineering; California Institute of Technology (CalTech), Pasadena, CA (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis. Division of Chemistry and Chemical Engineering
California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis. Division of Chemistry and Chemical Engineering; Univ. of California, Irvine, CA (United States). Dept. of Chemistry
Univ. of California, Irvine, CA (United States). Dept. of Chemistry

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). Additionally, 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.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0004993

OSTI ID:: 1850862

Alternate ID(s):: OSTI ID: 1811151

Journal Information:: Journal of Electroanalytical Chemistry, Journal Name: Journal of Electroanalytical Chemistry Journal Issue: C Vol. 875; ISSN 1572-6657

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Reprint of "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"

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References (23)

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