Abstract
High-sensitivity and wide-frequency attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) is highly demanded in unraveling electrocatalytic processes at the molecular level. In this work, an in situ ATR-SEIRAS technique incorporating a micromachined Si wafer window, p-polarized infrared radiation, and isotope labeling is extended to revisit the acetaldehyde oxidation reaction (AOR) on a Pt electrode in an acidic medium. New spectral features in the fingerprint region are detected, including ω(C-H) at 1078 cm-1 and νas(C-C-O) at 919 cm-1 for adsorbed acetaldehyde and δ(O-C-O) at 689 cm-1 for adsorbed acetate, besides the other enhanced and clearly discriminated spectral signals at higher frequencies. Time-evolved and potential-dependent ATR-SEIRAS measurements together with advanced density functional theory calculations considering the coadsorption of CO and C2 species enable clarification of the structures and roles of surface C2 intermediates (η1(C)-acetyl and η1(H)-acetaldehyde), as reflected by the two bands at 1630 and 1663 cm-1, respectively, leading to updated pathways for the AOR on a Pt electrode.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
