Regulating the product distribution of CO reduction by the atomic-level structural modification of the Cu electrode surface

Kim, Youn -Geun; Javier, Alnald; Baricuatro, Jack H.; Soriaga, Manuel P.

doi:10.1007/s12678-016-0314-1

Regulating the product distribution of CO reduction by the atomic-level structural modification of the Cu electrode surface

Journal Article · Tue Jun 07 04:00:00 EDT 2016 · Electrocatalysis

DOI:https://doi.org/10.1007/s12678-016-0314-1· OSTI ID:1333925

Kim, Youn -Geun ^[1]; Javier, Alnald ^[2]; Baricuatro, Jack H. ^[2]; Soriaga, Manuel P. ^[3]

California Institute of Technology, Pasadena, CA (United States); California Institute of Technology
California Institute of Technology, Pasadena, CA (United States)
California Institute of Technology, Pasadena, CA (United States); Texas A & M Univ., College Station, TX (United States)

Here, Cu catalyzes the electrochemical reduction of CO₂ or CO to an assortment of products, a behavior that is a detriment when only one reduced compound is desired. The present article provides an example in which, through the atomic-level control of the structure of the Cu electrode surface, the yield distribution is regulated to generate only one product. The reaction investigated was the preferential reduction of CO to C₂H₅OH on Cu at a low overpotential in alkaline solution. Experimental measurements combined electrochemical scanning tunneling microscopy (ECSTM) and differential electrochemical mass spectrometry (DEMS). An atomically ordered Cu(100) surface, prepared from either a single crystal or by Cu(pc)-to-Cu(100) reconstruction, did not produce ethanol. When the surfaces were subjected to monolayer-limited Cu↔Cu₂O cycles, only the reconstructed surface underwent an additional structural transformation that spawned the selective production of ethanol at a potential 645 mV lower than that which generates multiple products. Quasi-operando ECSTM indicated transformation to an ordered stepped surface, Cu(S) [3(100)×(111)], or Cu(511). The non-selective, multiple-product Cu-catalyzed reduction of CO had thus been regulated to yield only one liquid fuel by an atomic-level structural modification of the electrode surface.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

DOE Contract Number:: SC0004993

OSTI ID:: 1333925

Journal Information:: Electrocatalysis, Journal Name: Electrocatalysis Journal Issue: 5 Vol. 7; ISSN 1868-2529

Publisher:: Springer

Country of Publication:: United States

Language:: English

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