Model Studies on Heterogeneous Catalysts at the Atomic Scale

Freund, Hans‐Joachim; Shaikhutdinov, Shamil K.; Nilius, Niklas

doi:10.1007/s11244-014-0276-6

Cited by 9 publications

(5 citation statements)

References 43 publications

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“…This interpretation is also supported by the presence of a strong peak in STS spectra detected at about 0.25 eV below E F , very similar to the resonance observed in spectra acquired on invar alloys [259]. 1 4.3. Growth of metallic buffer layers on Fe(001) and Fe(001…”

Section: Wetting Layer Oxides On Fe(001)supporting

confidence: 78%

“…Interface formation between metals and oxides are one of the most widely investigated topic in physics, chemistry and material science. The reason for this huge interest is that there is almost no technological field in which the metal-oxide interaction does not play a prominent role, including (nano) catalysis [1][2][3], microelectronics [4,5], magnetic storage media [6], and protective coatings against corrosion [7,8].…”

Section: Introductionmentioning

confidence: 99%

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Reactive metal–oxide interfaces: A microscopic view

Picone

Riva

Brambilla

et al. 2016

Surface Science Reports

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Metal-oxide interfaces play a fundamental role in determining the functional properties of artificial layered heterostructures, which are at the root of present and future technological applications. Magnetic exchange and magnetoelectric coupling, spin filtering, metal passivation, catalytic activity of oxide-supported nano-particles are just few examples of physical and chemical processes arising at metal-oxide hybrid systems, readily exploited in working devices. These phenomena are strictly correlated with the chemical and structural characteristics of the metal-oxide interfacial region, making a thorough understanding of the atomistic mechanisms responsible of its formation a prerequisite in order to tailor the device properties. The steep compositional gradient established upon formation of metal-oxide heterostructures drives strong chemical interactions at the interface, making the metal-oxide boundary region a complex system to treat, both from an experimental and a theoretical point of view. However, once properly mastered, interfacial chemical interactions offer a further degree of freedom for tuning the material properties. The goal of the present review is to provide a summary of the latest achievements in the understanding of metal/oxide and oxide/metal layered systems characterized by reactive interfaces. The influence of the interface composition on the structural, electronic and magnetic properties will be highlighted. Particular emphasis will be devoted to the discussion of ultra-thin epitaxial oxides stabilized on highly oxidizable metals, which have been rarely exploited as oxide supports as compared to the much more widespread noble and quasi noble metallic substrates. In this frame, an extensive discussion is devoted to the microscopic characterization of interfaces between epitaxial metal oxides and the Fe(001) substrate, regarded from the one hand as a prototypical ferromagnetic material and from the other hand as a highly oxidizable metal.

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Section: Wetting Layer Oxides On Fe(001)supporting

confidence: 78%

Section: Introductionmentioning

confidence: 99%

Reactive metal–oxide interfaces: A microscopic view

Picone

Riva

Brambilla

et al. 2016

Surface Science Reports

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“…A mechanistic understanding of catalytic processes on solid surfaces requires to reveal the correlative relationship between the catalyst structure and the reaction kinetics over a wide range of the length scales. On the nm-scale, the surface structure controls the adsorption, diffusion and interaction of adsorbates [1][2][3]. Catalytic light-off is initiated on the nm-scale as well [4], but proceeds by propagation of reaction fronts via the meso-to the macro-scale [5,6].…”

Section: Introductionmentioning

confidence: 99%

Catalysis by Imaging: From Meso- to Nano-scale

Suchorski

Rupprechter

2020

Top Catal

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In-situ imaging of catalytic reactions has provided insights into reaction front propagation, pattern formation and other spatio-temporal effects for decades. Most recently, analysis of the local image intensity opened a way towards evaluation of local reaction kinetics. Herein, our recent studies of catalytic CO oxidation on Pt(hkl) and Rh(hkl) via the kinetics by imaging approach, both on the meso- and nano-scale, are reviewed. Polycrystalline Pt and Rh foils and nanotips were used as µm- and nm-sized surface structure libraries as model systems for reactions in the 10–5–10–6 mbar pressure range. Isobaric light-off and isothermal kinetic transitions were visualized in-situ at µm-resolution by photoemission electron microscopy (PEEM), and at nm-resolution by field emission microscopy (FEM) and field ion microscopy (FIM). The local reaction kinetics of individual Pt(hkl) and Rh(hkl) domains and nanofacets of Pt and Rh nanotips were deduced from the local image intensity analysis. This revealed the structure-sensitivity of CO oxidation, both in the light-off and in the kinetic bistability: for different low-index Pt surfaces, differences of up to 60 K in the critical light-off temperatures and remarkable differences in the bistability ranges of differently oriented stepped Rh surfaces were observed. To prove the spatial coherence of light-off on nanotips, proper orthogonal decomposition (POD) as a spatial correlation analysis was applied to the FIM video-data. The influence of particular configurations of steps and kinks on kinetic transitions were analysed by using the average nearest neighbour number as a common descriptor. Perspectives of nanosized surface structure libraries for future model studies are discussed.

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“…Even the remarkable effect of dopants and impurities in oxides may now be addressed. 5 While surface science has proven to be useful for a wide variety of catalytic processes, reactions on the most abundantly used catalysts, namely zeolites, remained a challenge due to the lack of suitable model systems mimicking zeolites. Basically, there is a simple reason for this.…”

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confidence: 99%

Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations

Boscoboinik

Shaikhutdinov

2014

Catal Lett

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The complexity of catalysts that the surface science community has been able to address has increased substantially in a systematic manner, starting with metal and oxide single crystal surfaces and evolving to an atomistic description of clusters and nanoparticles on well-defined, planar supports. The next step in adding complexity is now to address surfaces of porous oxide materials, in particular of zeolites, which are the most extensively used catalysts in the industry. The recently reported successful fabrication of well-ordered thin films, consisting of planar arrangement of aluminosilicate polygonal prisms on a metal substrate counting with highly acidic bridging hydroxyl groups on the surface, represents the limiting case of infinitely large pore and cages in zeolites. This model system allows one to study reactions catalyzed by zeolites using the toolkit of surface science. In this Perspective, we describe the zeolitic model system, with its virtues and limitations, as well as the challenges, opportunities and expectations for the future in modelling porous catalysts by a surface science approach.

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Model Studies on Heterogeneous Catalysts at the Atomic Scale

Cited by 9 publications

References 43 publications

Reactive metal–oxide interfaces: A microscopic view

Reactive metal–oxide interfaces: A microscopic view

Catalysis by Imaging: From Meso- to Nano-scale

Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations

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