Probing boundary sites on a Pt/Al2O3 model catalyst by CO2 hydrogenation and in situATR-IR spectroscopy of catalytic solid–liquid interfaces

文献信息

发布日期 2002-05-09
DOI 10.1039/B111498K
影响因子 3.676
作者

Davide Ferri, Thomas Bürgi, Alfons Baiker


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摘要

In situ ATR infrared spectroscopy was used to follow the reaction of CO2 with hydrogen at the solid–liquid interface of a model Pt/Al2O3 catalyst in cyclohexane at 313 K. CO2 adsorbs on Al2O3 to form carbonate-like species, which react with hydrogen to form CO. The observed spectrum exhibits unusually low vibrational frequencies and ratio of linearly to bridged bonded CO. In contrast, CO adsorbed from the solution onto the Pt/Al2O3 model catalyst results in a normal spectrum for CO on Pt. The results suggest that the reaction of CO2 and hydrogen takes place at the boundary sites of the interface between the Pt and the Al2O3 and that the resulting CO selectively probes these sites. The unusual CO spectrum indicates that these sites are characterised by a low ionisation potential of the d-valence orbitals of Pt. It is likely that the unusual property of these Pt sites are caused by a nearby oxygen vacancy of the Al2O3, onto which the CO2 initially adsorbs.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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