CO2 electrochemical reduction at thiolate-modified bulk Au electrodes

Fang, Yuxin; Cheng, Xun; Flake, John C.; Xu, Ye

doi:10.1039/c9cy00506d

Title: CO₂ electrochemical reduction at thiolate-modified bulk Au electrodes

Journal Article · Tue Apr 23 00:00:00 EDT 2019 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/c9cy00506d· OSTI ID:1577571

Fang, Yuxin ^[1]; Cheng, Xun ^[1]; Flake, John C. ^[1];

^[1]

Louisiana State Univ., Baton Rouge, LA (United States)

Electrochemical reduction provides an opportunity to convert atmospheric CO₂ to fuels or chemicals using renewable energy. Here, we demonstrate unexpected influence on the catalytic activity and selectivity of the electrochemical CO₂ reduction reaction (CO₂RR) through the functionalization of Au with thiols. 2-Phenylethanethiol modified Au electrodes (2-PET-Au) show up to a 2-fold enhancement in both Faradaic efficiency and current density for CO evolution, between –0.6 and –0.9 V vs. the reversible hydrogen electrode. Functionalization with 2-mercaptopropionic acid, which has a readily ionized carboxylate group, leads to hydrogen evolution with up to 100% Faradaic efficiency at the expense of CO evolution. Remarkably, the adsorption of certain thiols on Au does not have a negative impact on the total current density compared to blank Au. We present evidence that it is due to ligand-induced reconstruction of Au surfaces resulting in the creation of structurally and chemically modified local reaction environments. Thus a thiol species such as 2-PET, which does not contain any nitrogen-based heterocycle with a charge transfer center, can induce the formation of active sites on Au that are electrochemically active toward CO₂RR within the range of electrode potential that most of the ligand concentration remains stable on Au. Our findings suggest a simple, effective, and tunable way to modify the activity and selectivity of Au electrodes.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; CBET-1438385

OSTI ID:: 1577571

Alternate ID(s):: OSTI ID: 1510369

Journal Information:: Catalysis Science and Technology, Vol. 9, Issue 10; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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