The infrared (IR) chemiluminescence spectra of CO2 were measured during the steady-state CO + O2 reaction over Pt(110) and Pt(111) surfaces. Analysis of the IR emission spectra indicates that the bending vibrational temperature (TVB), as well as the antisymmetric vibrational temperature (TVAS), was higher on Pt(110) than on Pt(111). On the Pt(110) surface, the highly excited bending vibrational mode compared to the antisymmetric vibrational mode was observed under reaction conditions at low CO coverage (theta(CO) < 0.2) or at high surface temperatures (TS > or = 700 K). This can be related to the activated complex of CO2 formation in a more bent form on the inclined (111) terraces of the Pt(110)(1 x 2) structure. On the other hand, at high CO coverage (theta(CO) > 0.2) or at low surface temperatures (TS < 650 K), TVAS was higher than TVB, which can be caused by the reconstruction of the Pt(110)(1 x 2) surface to the (1 x 1) form with high CO coverage.
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http://dx.doi.org/10.1021/jp054829h | DOI Listing |
Materials (Basel)
November 2024
Department of Electrochemistry, Institute of Chemistry, Technology and Metallurgy, University of Belgrade, Njegoševa 12, 11000 Belgrade, Serbia.
J Phys Chem C Nanomater Interfaces
September 2024
Leiden Institute of Chemistry, Leiden University, Leiden 2333 CC, The Netherlands.
Hydrogen adsorption on platinum (Pt) single-crystal electrodes has been studied intensively in both experiments and computations. Yet, the precise origin and nature of the repulsive interactions observed between hydrogen adsorbates (H) have remained elusive. Here, we use first-principles density functional theory calculations to investigate in detail the interactions between H on Pt(111), Pt(100), and Pt(110) surfaces.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
May 2024
Department of Chemical Engineering and Materials Science, Stevens Institute of Technology, Hoboken, New Jersey 07030, United States.
Within computational heterogeneous catalysis, two critical factors exist-coverage and multifaceted effects-which are challenging to incorporate and contribute to differences between the results obtained from computational and experimental studies. Such disparities exist when significant adsorbate-adsorbate interactions are present, particularly when coupled with computationally limited facet sampling. Here, we designed a study to demonstrate the significance of coverage and facet effects on the predicted coverages for O* and H* on Pt nanoparticles.
View Article and Find Full Text PDFPhys Chem Chem Phys
April 2024
Institute of Materials Innovation, Institutes of Innovation for Future Society, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8601, Japan.
Developing innovative platinum-based electrocatalysts and enhancing their efficiency are crucial for advancing high-performance fuel cell technology. In this study, we employed DFT calculations to provide a theoretical basis for interpreting the impact of graphene coatings on various Pt surfaces on oxygen reduction reaction (ORR) catalytic activity, which are currently applied as protective layers in experiments. We comprehensively assess the geometric and electronic properties of Pt(100), Pt(110), and Pt(111) surfaces in comparison to their graphene-coated counterparts, revealing different adsorption behaviors of O across these surfaces.
View Article and Find Full Text PDFJ Phys Chem Lett
March 2024
Interface Research and Catalysis, ECRC, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstraße 3, 91058 Erlangen, Germany.
Electrochemically active liquid organic hydrogen carriers (EC-LOHCs) can be used directly in fuel cells; so far, however, they have rather low hydrogen storage capacities. In this work, we study the electrooxidation of a potential EC-LOHC with increased energy density, 1-cyclohexylethanol, which consists of two storage functionalities (a secondary alcohol and a cyclohexyl group). We investigated the product spectrum on low-index Pt single-crystal surfaces in an acidic environment by combining cyclic voltammetry, chronoamperometry, and in situ infrared spectroscopy, supported by density functional theory.
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