Engineering of Transition Metal Catalysts Confined in Zeolites

Kosinov, Nikolay; Liu, Chong; Hensen, Emiel J. M.; Pidko, Evgeny A.

doi:10.1021/acs.chemmater.8b01311

Cited by 266 publications

(190 citation statements)

References 263 publications

(361 reference statements)

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“…[83] Part of the metal is present as well-defined species and for those species some characterization techniques useful for supported organometallic compounds can be insightful for the metal on HZSM-5 system as well. [71,84] Both CO FTIR and 13 C MAS NMR are often used to characterize metal-organics supported on silica. CO FTIR can distinguish between mono-or dimeric and species and bigger clusters.…”

Section: Mnmentioning

confidence: 99%

“…It is likely that the confinement effect of the zeolite also stabilizes mono-and dimeric species at the OH-groups inside the porous structure of the zeolite. [84] Because of this, they can direct the cation to take on many different geometries. [65] This complicates characterization further, because it leads to rather broad contributions for spectroscopic techniques that probe the metal directly like EPR, [94,95] 95 Mo NMR, [96] UV-Vis, [67,68,97] XAS, [98] UV-Raman [79,99] and XPS [7,100] .…”

Section: Mnmentioning

confidence: 99%

“…For other metals, using chemical vapor deposition (CVD) techniques or cation exchange to incorporate the metal leads to better dispersion compared to the predominantly used solid ion exchange (SIE) and Incipient Wetness Impregnation (IWI). [84,102] CVD was performed for MDA using WCl 6 , but it is not known, if this improved the 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 dispersion of the metal, because the catalyst synthesized this way was not compared to a catalyst prepared with the conventional method of IWI. [75] For zeolites with bigger cages, Mo(CO) 6 is often incorporated into the zeolite through CVD.…”

Section: Mnmentioning

confidence: 99%

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Progress in Developing a Structure‐Activity Relationship for the Direct Aromatization of Methane

et al. 2018

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To secure future supply of aromatics, methane is a commercially interesting alternative feedstock. Direct conversion of methane into aromatics combines the challenge of activating one of the strongest C−H bonds in all hydrocarbons with the selective aromatization over zeolites. To address these challenges, smart catalyst and process design are a must. And for that, understanding the most important factors leading to successful methane C−H bond activation and selective aromatization is needed. In this review, we summarize mechanistic insight that has been gained so far not only for this reaction, but also for other similar processes involving aromatization reactions over zeolites. With that, we highlight what can be learnt from similar processes. In addition, we provide an overview of characterization tools and strategies, which are useful to gain structural information about this particular metal‐zeolite system at reaction conditions. Here we also aim to inspire future characterization work, by giving an outlook on characterization strategies that have not yet been applied for the methane dehydroaromatization catalyst, but are promising for this system.

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Section: Mnmentioning

confidence: 99%

Section: Mnmentioning

confidence: 99%

Section: Mnmentioning

confidence: 99%

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Progress in Developing a Structure‐Activity Relationship for the Direct Aromatization of Methane

et al. 2018

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“…Engineering of defined transition metal catalysts confined in zeolite pores has been recently reviewed in ref. [11]. Such species can bring about new catalytic functionalities expanding thus the scope of application of the zeolite catalysts.…”

Section: Introductionmentioning

confidence: 99%

The Nature and Catalytic Function of Cation Sites in Zeolites: a Computational Perspective

Pidko

2018

ChemCatChem

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110

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Zeolites have a broad spectrum of applications as robust microporous catalysts for various chemical transformations. The reactivity of zeolite catalysts can be tailored by introducing heteroatoms either into the framework or at the extraframework positions that gives rise to the formation of versatile Brønsted acid, Lewis acid and redox‐active catalytic sites. Understanding the nature and catalytic role of such sites is crucial for guiding the design of new and improved zeolite‐based catalysts. This work presents an overview of recent computational studies devoted to unravelling the molecular level details of catalytic transformations inside the zeolite pores. The role of modern computational chemistry in addressing the structural problem in zeolite catalysis, understanding reaction mechanisms and establishing structure‐activity relations is discussed. Special attention is devoted to such mechanistic phenomena as active site cooperativity, multifunctional catalysis as well as confinement‐induced and multisite reactivity commonly encountered in zeolite catalysis.

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“…Due to the nature of a heterogeneous catalyst, synthesizing a metal‐zeolite composite catalyst with homogeneous distribution of the active phase is challenging. Heterogeneity of the catalyst increases the difficulty of characterization and data interpretation, which can be seen for a recently developed synthesis technique that deposits transition metals within hollow zeolites . Because the active metal phase is located within the zeolite shell, this catalyst can serve as a multifunctional nanoreactor, with many applications including selective hydrogenation.…”

Section: Discussionmentioning

confidence: 99%

Characterization of Metal‐zeolite Composite Catalysts: Determining the Environment of the Active Phase

et al. 2020

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Metal‐zeolite composite catalysts are attracting increased attention due to their unique multifunctional properties. However, it is challenging to identify the physicochemical environment of the active phase, which is essential to improve our understanding of the structure‐performance relationships of such complex catalysts. In this work, commonly available analytical techniques (FTIR, TEM, XRD, etc.) and state‐of‐the‐art user instrumentation (XAS, SANS, e‐TEM, etc.) are reviewed with respect to their applications at different stages of the catalyst lifetime, from early nucleation, to the reaction mechanism and deactivation. Each technique is discussed in detail with examples to provide suggestions and guidelines for choosing the characterization technique(s) that are most appropriate for determining the desired structure‐property relationships of metal‐zeolite composite catalysts. Understanding the most appropriate applications of characterization techniques promotes development of novel synthesis methodologies, and in turn, applications for designing active, selective and stable multifunctional metal‐zeolite composite catalysts.

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Engineering of Transition Metal Catalysts Confined in Zeolites

Cited by 266 publications

References 263 publications

Progress in Developing a Structure‐Activity Relationship for the Direct Aromatization of Methane

Progress in Developing a Structure‐Activity Relationship for the Direct Aromatization of Methane

The Nature and Catalytic Function of Cation Sites in Zeolites: a Computational Perspective

Characterization of Metal‐zeolite Composite Catalysts: Determining the Environment of the Active Phase

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