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http://dx.doi.org/10.1002/anie.200702868 | DOI Listing |
J Phys Chem C Nanomater Interfaces
August 2025
University of Innsbruck, Innrain 52c, Innsbruck 6020, Austria.
Gold (Au), especially single-crystalline Au(111), has been extensively studied in fundamental electrochemistry due to its unique properties, including high conductivity, chemical stability, and well-defined surface characteristics, which make it an ideal model system for electrochemical investigations. At the same time, the Au(111) surface is known to degrade during oxidation-reduction cycling in commonly used electrolytes, exhibiting the formation of atomic-scale vacancy and adatom islands. Although there are many fundamental studies on these degradation processes, only a limited number of studies have been performed in alkaline media.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241000, P.R. China.
The control of surface and interface structures in nanocatalysts is a promising strategy for enhancing catalytic performance, but significant challenges persist in achieving precisely designed active sites or environments on the surface/interface of fully protected metal nanoclusters. In this study, we report the construction of an exposed Au atom on Au(111) and the formation of a unique surface/interface environment on the Au cluster via a cyclopentanethiol-etching strategy. Theoretical calculations and in situ attenuated total reflection infrared adsorption spectroscopy reveal that the exposed Au atom facilitates CO activation, while the tailored surface/interface environment promotes the accumulation of strongly hydrogen-bonded water, which can be validated by the molecular dynamic simulation, thus enhancing proton transfer and suppressing hydrogen evolution reaction (HER).
View Article and Find Full Text PDFPrecis Chem
March 2025
Hefei National Research Center for Physical Sciences at Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China.
Understanding how the electrolyte pH affects electrocatalytic activity is a topic of crucial importance in a large variety of systems. However, unraveling the origin of the pH effects is complicated often by the fact that both the reaction driving forces and reactant concentrations in the electric double layer (EDL) change simultaneously with the pH value. Herein, we employ the hydrogen evolution reaction (HER) at Au(111)-aqueous solution interfaces as a model system to disentangle different pH-dependent factors.
View Article and Find Full Text PDFPhys Rev Lett
January 2025
Huazhong University of Science and Technology, State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Wuhan 430074, China.
Constant-potential molecular dynamics (MD) simulations are indispensable for understanding the structure, capacitance, and dynamics of electrical double layers (EDLs) at the atomistic level. However, the classical constant-potential method, relying on the so-called "fluctuating charges" to keep electrode equipotential, overlooks quantum effects on the electrode and always underestimates EDL capacitance for typical metal electrode and aqueous electrolyte interfaces. Here, we propose a constant potential method accounting for electron spillover on the outermost nuclei of the electrode.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
November 2024
Leiden Institute of Chemistry, Leiden University, PO Box 9502, 2300 RA Leiden, The Netherlands.
Oxidation-reduction cycles (ORCs) on Au(111) in 0.1 M sulfuric acid solution change the electrode morphology due to the formation of many new nanosized islands. With increasing the cycle number, the roughness of the surface increases due to the formation of multiatomic-step adatom islands and pits.
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