Quantized Electrodes: Atomic Palladium and Gold in Polyaniline

McDaniel, Jesse G.; Josowicz, Mira; Janata, Jiří

doi:10.1002/celc.202100281

Quantized Electrodes: Atomic Palladium and Gold in Polyaniline

Journal Article · Tue Mar 30 00:00:00 EDT 2021 · ChemElectroChem

DOI:https://doi.org/10.1002/celc.202100281· OSTI ID:1786190

McDaniel, Jesse G. ^[1]; Josowicz, Mira ^[1]; Janata, Jiří ^[1]

School of Chemistry and Biochemistry Georgia Institute of Technology 901 Atlantic Dr. Atlanta GA 30332 USA

Abstract

Electrochemically deposited Pd _m Au _n metal clusters on a polyaniline‐coated Pt electrode have been shown to exhibit an “ordering effect”, in which the catalytic activity for n‐propanol oxidation depends sensitively on the precise order that the metal atoms are deposited. For example, tri‐atomic Pd ₂ Au clusters exhibit different catalytic activity for electrodeposition order Pd−Pd−Au compared to Pd−Au−Pd on the polyaniline (PANI)/Pt matrix. In this work, we utilize density functional theory (DFT) to elucidate the structure and energetics of tri‐atomic Pd _m Au _n clusters attached to a model PANI support. We provide a rationale for the experimentally observed “ordering effect” in terms of specific covalent interactions between the metal atoms and PANI framework that alter the net stability of the metal catalyst. We find that hydroxyl radical binding energies computed for the model catalytic systems provide a good descriptor for the experimentally measured catalytic activity for n‐propanol oxidation. In addition, the good correlation between experiment/theory serves as additional confirmation of our proposed catalytic structures and rationale of the previously unexplained “ordering effect”. Our study highlights the important role of the PANI support in determining the activity of uniquely‐defined, atomic metal catalysts.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0020279

OSTI ID:: 1786190

Alternate ID(s):: OSTI ID: 1853542

Journal Information:: ChemElectroChem, Journal Name: ChemElectroChem Journal Issue: 10 Vol. 8; ISSN 2196-0216

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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