Homogeneous and Heterogeneous Catalysis: Bridging the Gap Through Surface Organometallic Chemistry

Copéret, Christophe; Chabanas, Mathieu; Saint‐Arroman, Romain Petroff; Basset, Jean‐Marie

doi:10.1002/chin.200316246

Cited by 13 publications

(15 citation statements)

References 40 publications

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“…[1][2][3][4] Both heterogeneous porous hosts and homogeneous templates have been used as support for M NPs. [5][6][7][8][9][10][11][12][13][14][15][16] For example, metal-organic frameworks (MOFs), 6 covalent organic frameworks (COFs), 7 porous organic polymers (POPs), 8,9 organic cages, 10 and ionic liquids 11 are all commonly applied to encapsulate M NPs. As a result, M NP/support composites are widely used for catalysis because the space confinement effect of these supports increases substrate selectivity and improves the catalytic activity as a result of enhanced exposure of active centers.…”

Section: Introductionmentioning

confidence: 99%

Ultra-Small Face-Centered-Cubic Ru Nanoparticles Confined within a Porous Coordination Cage for Dehydrogenation

Fang

Togo

et al. 2018

Chem

130

101

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Porous coordination cages (PCCs) are discrete nanoscopic structures with intrinsic cavities. The solubility and tunable host-guest interactions allow PCCs to form a homogeneous catalytic platform. Through engineering the interactions between the host PCC and the guest nanoparticles, we succeeded in encapsulating ruthenium nanoparticles in PCCs and tuning their crystalline form to a highly reactive face-centered-cubic one. The nanoparticles within the PCC showed extraordinary reactivity toward the dehydrogenation reaction. This approach sheds light on developing high-performance catalysts through interaction engineering.

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Section: Introductionmentioning

confidence: 99%

Ultra-Small Face-Centered-Cubic Ru Nanoparticles Confined within a Porous Coordination Cage for Dehydrogenation

Fang

Togo

et al. 2018

Chem

130

101

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“…Recent investigations on supported metallocene catalysts based on smectite supports have been reported [ 23 , 24 ]. It is known that the acidic properties of these materials may influence the type of interaction with the metallocene complex and its activation process, with consequent effects on overall productivity [ 41 , 42 , 43 ]. These clay materials have Lewis and Brönsted acidic sites and their actuation to generate the active species could be argued in two ways, similar to the homogeneous systems.…”

Section: Resultsmentioning

confidence: 99%

Silicoaluminates as “Support Activator” Systems in Olefin Polymerization Processes

et al. 2010

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In this work we report the polymerization behaviour of natural clays (montmorillonites, MMT) as activating supports. These materials have been modified by treatment with different aluminium compounds in order to obtain enriched aluminium clays and to modify the global Brönsted/Lewis acidity. As a consequence, the intrinsic structural properties of the starting materials have been changed. These changes were studied and these new materials used for ethylene polymerization using a zirconocene complex as catalyst. All the systems were shown to be active in ethylene polymerization. The catalyst activity and the dependence on acid strength and textural properties have been also studied. The behaviour of an artificial silica (SBA 15) modified with an aluminium compound to obtain a silicoaluminate has been studied, but no ethylene polymerization activity has been found yet.

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“…Molecules on surfaces 1 , 2 offer a great variability of creating functional structures for future technologies 3 – 5 , including molecular electronics 6 , 7 , data storage 8 , 9 , sensing 10 , and catalysis 11 , 12 . This is particularly true when considering molecules that carry or coordinate metal atoms, e.g., in structures formed from metalated molecules such as metaloporphyrins 13 and metalocyanines 14 as well as surface-supported metal–organic frameworks 15 , 16 or metal–organic coordination networks 17 .…”

Section: Introductionmentioning

confidence: 99%

“…This is particularly true when considering molecules that carry or coordinate metal atoms, e.g., in structures formed from metalated molecules such as metaloporphyrins 13 and metalocyanines 14 as well as surface-supported metal–organic frameworks 15 , 16 or metal–organic coordination networks 17 . All these structures offer additional interesting magnetic and superior catalytic 11 activities 15 , 18 – 20 . Creating functional molecular structures on surfaces is based on the capability to anchor molecules to specific adsorption sites under operation condition, i.e., ideally at room temperature.…”

Section: Introductionmentioning

confidence: 99%

Creating a regular array of metal-complexing molecules on an insulator surface at room temperature

et al. 2020

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Controlling self-assembled nanostructures on bulk insulators at room temperature is crucial towards the fabrication of future molecular devices, e.g., in the field of nanoelectronics, catalysis and sensor applications. However, at temperatures realistic for operation anchoring individual molecules on electrically insulating support surfaces remains a big challenge. Here, we present the formation of an ordered array of single anchored molecules, dimolybdenum tetraacetate, on the (10.4) plane of calcite (CaCO3). Based on our combined study of atomic force microscopy measurements and density functional theory calculations, we show that the molecules neither diffuse nor rotate at room temperature. The strong anchoring is explained by electrostatic interaction of an ideally size-matched molecule. Especially at high coverage, a hard-sphere repulsion of the molecules and the confinement at the calcite surface drives the molecules to form locally ordered arrays, which is conceptually different from attractive linkers as used in metal-organic frameworks. Our work demonstrates that tailoring the molecule-surface interaction opens up the possibility for anchoring individual metal-complexing molecules into ordered arrays.

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Homogeneous and Heterogeneous Catalysis: Bridging the Gap Through Surface Organometallic Chemistry

Cited by 13 publications

References 40 publications

Ultra-Small Face-Centered-Cubic Ru Nanoparticles Confined within a Porous Coordination Cage for Dehydrogenation

Ultra-Small Face-Centered-Cubic Ru Nanoparticles Confined within a Porous Coordination Cage for Dehydrogenation

Silicoaluminates as “Support Activator” Systems in Olefin Polymerization Processes

Creating a regular array of metal-complexing molecules on an insulator surface at room temperature

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