CO oxidation trends on Pt-group metals from ultrahigh vacuum to near atmospheric pressures: A combined in situ PM-IRAS and reaction kinetics study

Gao, Feng; McClure, Sean M.; Cai, Yun; Gath, Kerrie; Wang, Y.; Chen, Mingshu; Guo, Qiangsheng; Goodman, D. W.

doi:10.1016/j.susc.2008.10.031

Cited by 110 publications

(101 citation statements)

References 22 publications

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“…CO oxidation is routinely used as the prototypical model reaction in heterogeneous catalysis research because it is seemingly simple, yet exhibits a variety of complex phenomena [27,28,31]. Highlights include Ertl's observation of temporal oscillations and spatial pattern formation on Pt(110) [27], Goodman's work on bridging the pressure gap on Pt-group metals [32], and Haruta's breakthrough discovery that nanoparticulate gold is highly active for CO oxidation even below room temperature [33,34]. This discovery undoubtedly marks the beginning of the 'gold rush' in heterogeneous catalysis leading to an astonishing > 5,000 papers published since 1987 and summarized in several review articles [34][35][36][37][38][39].…”

Section: Selective Oxidations Involving Carbon Monoxide (Co) and Hydrmentioning

confidence: 99%

Water-assisted oxygen activation during selective oxidation reactions

Tran

Doan

Chandler

et al. 2016

Current Opinion in Chemical Engineering

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Section: Selective Oxidations Involving Carbon Monoxide (Co) and Hydrmentioning

confidence: 99%

Water-assisted oxygen activation during selective oxidation reactions

Tran

Doan

Chandler

et al. 2016

Current Opinion in Chemical Engineering

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“…When moving from UHV conditions to elevated pressures, the effect of gas molecules close to the surface increases [5,6]. For example, a change of the gas composition can lead to compositional and structural changes of a working catalyst [7,8], which in turn can change the kinetics of the reaction.…”

Section: Introductionmentioning

confidence: 99%

Visualization of Gas Distribution in a Model AP-XPS Reactor by PLIF: CO Oxidation over a Pd(100) Catalyst

et al. 2017

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Abstract:In situ knowledge of the gas phase around a catalyst is essential to make an accurate correlation between the catalytic activity and surface structure in operando studies. Although ambient pressure X-ray photoelectron spectroscopy (AP-XPS) can provide information on the gas phase as well as the surface structure of a working catalyst, the gas phase detected has not been spatially resolved to date, thus possibly making it ambiguous to interpret the AP-XPS spectra. In this work, planar laser-induced fluorescence (PLIF) is used to visualize the CO 2 distribution in a model AP-XPS reactor, during CO oxidation over a Pd(100) catalyst. The results show that the gas composition in the vicinity of the sample measured by PLIF is significantly different from that measured by a conventional mass spectrometer connected to a nozzle positioned just above the sample. In addition, the gas distribution above the catalytic sample has a strong dependence on the gas flow and total chamber pressure. The technique presented has the potential to increase our knowledge of the gas phase in AP-XPS, as well as to optimize the design and operating conditions of in situ AP-XPS reactors for catalysis studies.

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“…Corresponding studies therefore often specifically target gas-phase conditions leading to highest catalytic activity. Such measurements are then prone to mass transfer limitations (MTLs) and concomitant significant variations in reactant and product concentrations inside the reactor chamber [9,[11][12][13][14][15] . In studies on flat-faced model catalysts, this is in particular the formation of a so-called boundary layer of product molecules above the catalyst surface, if these molecules are faster formed by the on-going reactions than can be transported away with the stream in the reactor [14][15] .…”

Section: Introductionmentioning

confidence: 99%

Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling

Matera

Blomberg²,

Hoffmann

et al. 2015

ACS Catal.

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We use multi-scale modeling to analyze laser-induced fluorescence (LIF) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density-functional theory based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIF signals we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions the experimental activity is due to pristine Pd(100), possibly coexisting with other (oxidic) domains on the surface.

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CO oxidation trends on Pt-group metals from ultrahigh vacuum to near atmospheric pressures: A combined in situ PM-IRAS and reaction kinetics study

Cited by 110 publications

References 22 publications

Water-assisted oxygen activation during selective oxidation reactions

Water-assisted oxygen activation during selective oxidation reactions

Visualization of Gas Distribution in a Model AP-XPS Reactor by PLIF: CO Oxidation over a Pd(100) Catalyst

Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling

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