Simultaneous Imaging of Gas Phase over and Surface Reflectance of a Pd(100) Single Crystal during CO Oxidation

Zhou, Jianfeng; Blomberg, Sara; Gustafson, Johan; Lundgren, Edvin; Zetterberg, Johan

doi:10.1021/acs.jpcc.7b08108

Cited by 23 publications

(33 citation statements)

References 37 publications

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“…This would build on previous studies where PLIF has been combined with 2D-SOR on single crystals. 16 , 17 It would then be possible to directly correlate a local change in the reflectivity with a local change in catalytic activity.…”

Section: Discussionmentioning

confidence: 99%

Operando Reflectance Microscopy on Polycrystalline Surfaces in Thermal Catalysis, Electrocatalysis, and Corrosion

Pfaff

Larsson

Orlov

et al. 2021

ACS Appl. Mater. Interfaces

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We have developed a microscope with a spatial resolution of 5 μm, which can be used to image the two-dimensional surface optical reflectance (2D-SOR) of polycrystalline samples in operando conditions. Within the field of surface science, operando tools that give information about the surface structure or chemistry of a sample under realistic experimental conditions have proven to be very valuable to understand the intrinsic reaction mechanisms in thermal catalysis, electrocatalysis, and corrosion science. To study heterogeneous surfaces in situ , the experimental technique must both have spatial resolution and be able to probe through gas or electrolyte. Traditional electron-based surface science techniques are difficult to use under high gas pressure conditions or in an electrolyte due to the short mean free path of electrons. Since it uses visible light, SOR can easily be used under high gas pressure conditions and in the presence of an electrolyte. In this work, we use SOR in combination with a light microscope to gain information about the surface under realistic experimental conditions. We demonstrate this by studying the different grains of three polycrystalline samples: Pd during CO oxidation, Au in electrocatalysis, and duplex stainless steel in corrosion. Optical light-based techniques such as SOR could prove to be a good alternative or addition to more complicated techniques in improving our understanding of complex polycrystalline surfaces with operando measurements.

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Section: Discussionmentioning

confidence: 99%

Operando Reflectance Microscopy on Polycrystalline Surfaces in Thermal Catalysis, Electrocatalysis, and Corrosion

Pfaff

Larsson

Orlov

et al. 2021

ACS Appl. Mater. Interfaces

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“…It is important that we can determine the spatial distribution of reactive species created in the volume of the plasma discharge especially those that exist close to the surface of the catalyst. Examples exist in the literature of the use of planar laser-induced fluorescence to determine such two-dimensional concentration profiles in plasma [21,22] and catalytic studies [23,24] and it would be timely to make such measurements in a suitable plasma-catalysis system. Such spatially resolved information will generate valuable insight and provide important information upon which theoretical modeling can be based.…”

Section: The Interaction Of Plasma and Catalystmentioning

confidence: 99%

Plasma-catalysis: Is it just a question of scale?

Whitehead

2019

Front. Chem. Sci. Eng.

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The issues of describing and understanding the changes in performance that result when a catalyst is placed into plasma are discussed. The different chemical and physical interactions that result and how their combination might produce beneficial results for the plasma-catalytic processing of different gas streams are outlined with particular emphasis being placed on the different range of spatial and temporal scales that must be considered both in experiment and modelling. The focus is on non-thermal plasma where the lack of thermal equilibrium creates a range of temperature scales that must be considered. This contributes in part to a wide range of inhomogeneity in different properties such as species concentrations and electric fields that must be determined experimentally by in situ methods and be incorporated into modelling. It is concluded that plasmacatalysis is best regarded as conventional catalysis perturbed by the presence of a discharge, which modifies its operating conditions, properties and outcomes often in a very localised way. The sometimes used description "plasma-activated catalysis" is an apt one.

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“…Consequently, this combination of integral activity measurements with single point probing of catalyst material state is prone to produce erroneous structure-function relationships 9,10 . In attempts to alleviate this problem, recent studies have used a combination of techniques to both spatially and temporally investigate model 3,[11][12][13][14][15][16][17] and more complex catalysts 9,11,12,[18][19][20][21][22] , with several comprehensive reviews on the topic published recently 2,9,10,23 . For example, the thin 150 μm capillary used in Spaci-MS 2 enables spatiotemporal characterization of reactant gradients with a spatial resolution of ca.…”

mentioning

confidence: 99%

Copper catalysis at operando conditions—bridging the gap between single nanoparticle probing and catalyst-bed-averaging

et al. 2020

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In catalysis, nanoparticles enable chemical transformations and their structural and chemical fingerprints control activity. To develop understanding of such fingerprints, methods studying catalysts at realistic conditions have proven instrumental. Normally, these methods either probe the catalyst bed with low spatial resolution, thereby averaging out single particle characteristics, or probe an extremely small fraction only, thereby effectively ignoring most of the catalyst. Here, we bridge the gap between these two extremes by introducing highly multiplexed single particle plasmonic nanoimaging of model catalyst beds comprising 1000 nanoparticles, which are integrated in a nanoreactor platform that enables online mass spectroscopy activity measurements. Using the example of CO oxidation over Cu, we reveal how highly local spatial variations in catalyst state dynamics are responsible for contradicting information about catalyst active phase found in the literature, and identify that both surface and bulk oxidation state of a Cu nanoparticle catalyst dynamically mediate its activity.

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Simultaneous Imaging of Gas Phase over and Surface Reflectance of a Pd(100) Single Crystal during CO Oxidation

Cited by 23 publications

References 37 publications

Operando Reflectance Microscopy on Polycrystalline Surfaces in Thermal Catalysis, Electrocatalysis, and Corrosion

Operando Reflectance Microscopy on Polycrystalline Surfaces in Thermal Catalysis, Electrocatalysis, and Corrosion

Plasma-catalysis: Is it just a question of scale?

Copper catalysis at operando conditions—bridging the gap between single nanoparticle probing and catalyst-bed-averaging

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