Enhanced Electrocatalytic Oxidation of Formic Acid on Au(111) in the Presence of Pyridine

Hermann, Johannes M.; Mattausch, Yannick; Weiß, Annchristin; Jacob, Timo; Kibler, Ludwig A.

doi:10.1149/2.0251815jes

Cited by 12 publications

(7 citation statements)

References 31 publications

(45 reference statements)

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“…First, the pyridyl group may directly interact with formic acid/formate, helping it to form an active intermediate for FAOR for understanding the role of pyridine (Py) on Au. 35,36 However, in our experiment of FAOR on Pt in the solution containing Py (seen in Figure S2.5 c), and its current measured is lower than that measured on Pt@4MPy. If Pt@4MPy follows the same reason, the FAOR may occur via chemical process followed by electrochemical process (CE).…”

Section: Resultscontrasting

confidence: 56%

Accelerated interfacial proton transfer for promoting electrocatalytic activity

Deng

Sun

et al. 2022

Chem. Sci.

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Section: Resultscontrasting

confidence: 56%

Accelerated interfacial proton transfer for promoting electrocatalytic activity

Deng

Sun

et al. 2022

Chem. Sci.

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“…Having a simple structure and multiple binding sites, pyridine is usually employed as a probe molecule for the investigation of complex electrochemical interface. More importantly, pyridine and its derivatives have been found to mediate some important electrochemical reactions, such as CO 2 reduction, − formic acid oxidation, , H 2 evolution, and oxidation. − Therefore, a delicate molecular-level understanding of the adsorption and reaction of pyridine at the electrochemical interface is quite meaningful.…”

Section: Introductionmentioning

confidence: 99%

Potential-Dependent Coadsorption of Pyridine Molecule and α-Pyridyl Radical at the Pt Electrode/Electrolyte Interface

et al. 2019

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Recently, attention on pyridine adsorption and reaction at the electrode/electrolyte interface has been revitalized in the context of pyridine-mediated reactions such as CO2 reduction. Taking Pt as an example, although numerous efforts have been made, disagreements are still unresolved regarding the potential-dependent adsorption of pyridine on the Pt electrode, which further prevents an explicit understanding of the pyridine-mediated electrochemical process at a molecular level. Here, we employed an operando electrochemical surface-enhanced Raman spectroscopy method, in combination with the density functional theory calculation and isotopic labeling of the molecule, to thoroughly study how pyridine interacts with the Pt electrode/electrolyte interface. For the first time, it is corroborated that pyridine is adsorbed on the Pt electrode in both pyridine molecule (Py) and α-pyridyl radical (α-Pyl) states. On the basis of a systematic investigation of the potential-dependent vibrational spectra, we further explored how the coverage, configuration, and binding strength of both Py and α-Pyl adsorbates on the Pt electrode are tuned by electrode polarization and accordingly established a structural model at the electrochemical interface. Our work not only ends the long-time disputes on how pyridine interacts with the Pt electrode but also provides crucial information for the mechanistic research of pyridine-mediated reaction process.

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“…The trend observed for this kink is in excellent agreement with the systematic series of sulfate spikes for Au in H2SO4 (Figure 3b). So far, this sudden change in the current for FAOR at 0.52 V has only been reported for large and well-ordered Au(111) single crystal surfaces [50,51]. This is a marked sign about the high-quality of the "Au(111)" electrodes through simple fabrication by cathodic corrosion.…”

Section: The Electrocatalytic Behavior Of Au After Cathodic Corrosionmentioning

confidence: 94%

An affordable option to Au single crystals through cathodic corrosion of a wire: Fabrication, electrochemical behavior, and applications in electrocatalysis and spectroscopy

Elnagar

Hermann

Jacob

et al. 2021

Electrochimica Acta

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Faceting and nanostructuring of polycrystalline gold electrodes by cathodic corrosion in concentrated potassium hydroxide electrolytes has been systematically studied at different electrode potentials. Current-potential curves for the restructured Au electrodes in 0.1 M H2SO4 show characteristic features of Au(111) facets in the double-layer and oxidation region.Thus, the modified Au electrodes adopt properties typically known for well-defined single crystal surfaces. Besides the preferential surface faceting, the electrochemically active surface area (EASA) is enhanced as a function of potential, concentration and time. Scanning electron micrographs show the formation of well-defined triangular pits and nanostructures with a specific orientation confirming the formation of (111)-facets. In this way, the behavior of single crystals is accompanied with the properties of nanoparticles which are of utmost interest in electrocatalysis and surface enhanced Raman spectroscopy (SERS). The electrocatalytic activity of the newly formed "Au(111)" surface from an Au wire has been tested towards the hydrogen evolution reaction (HER) and for the formic acid oxidation reaction (FAOR). The study of electrocatalytic reactions at these nanostructured electrodes allows to identify active centers, which are absent for extended single crystal surfaces.Adsorbed pyridine on the nanostructured Au electrodes directly shows SERS activity, while untreated polycrystalline Au is SERS-inactive. The use of cathodic corrosion of simple wires is a paradigm of SERS-applications in electrochemistry with clean Au electrodes that provide properties of Au(111) single crystals.

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Enhanced Electrocatalytic Oxidation of Formic Acid on Au(111) in the Presence of Pyridine

Cited by 12 publications

References 31 publications

Accelerated interfacial proton transfer for promoting electrocatalytic activity

Accelerated interfacial proton transfer for promoting electrocatalytic activity

Potential-Dependent Coadsorption of Pyridine Molecule and α-Pyridyl Radical at the Pt Electrode/Electrolyte Interface

An affordable option to Au single crystals through cathodic corrosion of a wire: Fabrication, electrochemical behavior, and applications in electrocatalysis and spectroscopy

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