Ligand-functionalized Pt nanoparticles as asymmetric heterogeneous catalysts: molecular reaction control by ligand–reactant interactions

Šulce, Anda; Backenköhler, Jana; Schrader, Imke; Piane, Massimo Delle; Müller, Christian; Wark, André; Ciacchi, Lucio Colombi; Azov, Vladimir A.; Kunz, Sebastian

doi:10.1039/c8cy01836g

Cited by 20 publications

(18 citation statements)

References 76 publications

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“…It was also observed that size had a strong effect on the catalytic activity, but not on the stereoselectivity gained by ligand functionalization for the hydrogenation of ethyl−acetoacetate [32] . More recent studies revealed that by utilizing specific ligand‐reactant interactions, even strong asymmetric biases can be achieved leading to enantiomeric excess of more than 80 % [42,43] …”

Section: Surfactant‐free Colloidal Synthesesmentioning

confidence: 99%

Beyond Active Site Design: A Surfactant‐Free Toolbox Approach for Optimized Supported Nanoparticle Catalysts

2021

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Developing new catalysts with superior activity, stability, and selectivity is the ultimate research goal in catalysis. However, a complete understanding of what makes new or already known supported catalysts performant is still challenging. In addition to a careful design of the catalytically active phase, properties such as the interparticle distance, the location of the active phase in the outer or inner pores of the support material, as well as preparation steps such as washing, storage conditions, and conditioning can severely affect the observed performance. With the example of supported Pt nanoparticles (NPs), it is illustrated how systematic studies, where only one experimental parameter is changed at a time independently of the others, provide detailed insights into supported heterogeneous catalyst design. To perform such studies, an integral toolbox approach based on a surfactant‐free colloidal synthesis of NPs is developed. This approach takes into account not only the design and production of the catalytically active phase but considers all steps prior to testing the catalyst. The toolbox is well suited to flag and address pitfalls beyond the active phase design, to study and optimize supported precious metal NPs for energy and chemical conversion processes.

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Section: Surfactant‐free Colloidal Synthesesmentioning

confidence: 99%

Beyond Active Site Design: A Surfactant‐Free Toolbox Approach for Optimized Supported Nanoparticle Catalysts

2021

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“…The modified catalysts were found to exhibit both improved selectivity and overall higher activity; the authors concluded that the ligand formed new reactive sites on the surface that facilitated H addition to the reactant. The same group has extended this approach to enantioselective hydrogenation of prochiral reactants, a field for which organic chiral modifiers have received significant attention . More recently still, Lari et al.…”

Section: Selective Surface Modificationmentioning

confidence: 99%

On‐the‐fly Catalyst Modification: Strategy to Improve Catalytic Processes Selectivity and Understanding

Sá

Medlin

2019

ChemCatChem

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Hydrogenation is a quintessential process to the chemical industry. It is heavily involved in organic synthesis and fuel production, among other processes. Preferentially the reactions are carried out with heterogeneous catalysts and when possible in flow mode. Herein, we provide a retrospective on selective surface modification of catalysts for improved selectivity and understanding of catalytic reactivity. In addition, we provide a prospectus for an emerging strategy of carrying out surface modification on-the-fly to produce novel catalysts in a fast and reproducible way and to understand catalytic phenomena.

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“…Mesoporous solid strong bases have drawn much attention in recent decades, because they can catalyze a series of reactions such as Michael addition, Knoevenagel condensation, and transesterification reaction in gentle conditions with few pollution issues . It is known that the high specific surface areas and the affluent porous structure of mesoporous solid strong bases are beneficial for rapid mass transfer and avert active site deactivation caused by carbon deposition that usually happens in microporous catalysts. − As heterogeneous catalysts, mesoporous solid bases present some advantages over liquid base catalysts, such as higher selectivity, easier separation, and better reusability. , Hence, numerous attempts have been made in the past decades to synthesize mesoporous solid strong bases for heterogeneous catalysis. − …”

Section: Introductionmentioning

confidence: 99%

Significant Decrease in Activation Temperature for the Generation of Strong Basicity: A Strategy of Endowing Supports with Reducibility

Peng

Lü

et al. 2019

Inorg. Chem.

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Mesoporous solid strong bases are quite attractive due to their good catalytic performance for applications as environmentally friendly catalysts in various reactions. However, pretty harsh conditions are usually compulsory for the fabrication of strong basicity by using traditional thermal activation (e.g., 700 °C for the activation of base precursor KNO3 supported on mesoporous Al2O3). This is energy intensive and harmful to the mesoporous structure. In this study, we report a strategy of endowing supports with reducibility (ESWR) by doping low-valence Cr3+ into mesoporous Al2O3, so that the activation temperature for basicity generation is decreased significantly. Fascinatingly, KNO3 on mesoporous Al2O3 can be motivated to basic sites completely at the temperature of 400 °C via the ESWR strategy, which is much lower than the conventional thermal activation (700 °C). We have demonstrated that the redox reciprocity between KNO3 and Cr3+ is responsible for the low-temperature conversion, and Cr6+ is formed quantitatively as the oxidation product. The obtained solid bases possessing ordered mesostructure and strong basicity provide promising candidates for base-catalyzed synthesis of dimethyl carbonate via transesterification. The catalytic activity is obviously higher than a typical solid base like MgO as well as a series of reported basic catalysts containing alkali metal and alkaline-earth metal oxides.

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Ligand-functionalized Pt nanoparticles as asymmetric heterogeneous catalysts: molecular reaction control by ligand–reactant interactions

Abstract: Stereoselective control on amino acid functionalized supported Pt nanoparticles by means of dispersion interactions.

Cited by 20 publications

References 76 publications

Beyond Active Site Design: A Surfactant‐Free Toolbox Approach for Optimized Supported Nanoparticle Catalysts

Beyond Active Site Design: A Surfactant‐Free Toolbox Approach for Optimized Supported Nanoparticle Catalysts

On‐the‐fly Catalyst Modification: Strategy to Improve Catalytic Processes Selectivity and Understanding

Significant Decrease in Activation Temperature for the Generation of Strong Basicity: A Strategy of Endowing Supports with Reducibility

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