Rotating Catalysts Are Superior: Suppressing Product Inhibition by Anchimeric Assistance in Four-Component Catalytic Machinery

Biswas, Pronay Kumar; Saha, Suman; Paululat, Thomas; Schmittel, Michael

doi:10.1021/jacs.8b04437

Cited by 49 publications

(65 citation statements)

References 28 publications

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“…Chemists are at the beginning of building synthetic catalysts with similar functions, with the long‐term aim to control chemical pathways in more complex chemical mixtures . In this context, there is increasing interest in synthetic catalysts that can be switched by external stimuli or cofactors . Most of these studies have been carried out using relatively simple hydrolysis reactions and organocatalytic reactions, and the number of transition‐metal catalysts that have a switching function is very limited .…”

Section: Figurementioning

confidence: 99%

Cofactor Controlled Encapsulation of a Rhodium Hydroformylation Catalyst

Jongkind

Elemans²,

Reek

2019

Angewandte Chemie

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Supramolecular approaches in transition‐metal catalysis, including catalyst encapsulation, have attracted considerable attention. Compared to enzymes, supramolecular catalysts in general are less complex. Enzyme activity is often controlled by the use of smaller cofactor molecules, which is important in order to control reactivity in complex mixtures of molecules. Interested in increasing complexity and allowing control over supramolecular catalyst formation in response to external stimuli, we designed a catalytic system that only forms an efficient supramolecular complex when a small cofactor molecule is added to the solution. This in turn affects both the activity and selectivity when applied in a hydroformylation reaction. This contribution shows that catalyst encapsulation can be controlled by the addition of a cofactor, which affects crucial catalyst properties.

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Section: Figurementioning

confidence: 99%

Cofactor Controlled Encapsulation of a Rhodium Hydroformylation Catalyst

Jongkind

Elemans²,

Reek

2019

Angewandte Chemie

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“…In another interesting example, coordination chemistry was used to prepare supramolecular nano-rotors where both the stator and the rotor are porphyrin derivatives connected by 1,4-diazabicyclo[2.2.2]octane (DABCO) as an axle between two porphyrin moieties, and two copper I ions ( Fig. 3) [24][25][26][27][28][29][30][31]. Variable temperature NMR analysis showed that the rotational speeds at 25 °C vary roughly from 0.5 to 100 kHz, mainly controlled by the rotor structure, solvent system, presence of Cu I , and addition of a suitable chelating agent.…”

Section: Sandwich-type Complexesmentioning

confidence: 99%

“…Interestingly, when the rotors were used as a catalyst for click reactions, the product yields correlated with the speed of the machine. The dependence of yield on rotation speed is attributed to the ability of a rotating catalyst to displace the product more efficiently from the active site [30].…”

Section: Sandwich-type Complexesmentioning

confidence: 99%

Heterocomponent ternary supramolecular complexes of porphyrins: A review

Prigorchenko

Ustrnul

Borovkov

et al. 2019

J. Porphyrins Phthalocyanines

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Porphyrins are prominent host molecules which are widely used due to their structural characteristics and directional interaction sites. This review summarizes non-covalently bound ternary complexes of porphyrins, constructed from at least three non-identical species. Progress in supramolecular chemistry allows the creation of complex molecular machinery tools, such as rotors, motors and switches from relatively simple structures in a single self-assembly step. In the current review, we highlight the collection of sophisticated molecular ensembles including sandwich-type complexes, cages, capsules, tweezers, rotaxanes, and supramolecular architectures mediating oxygen-binding and oxidation reactions. These diverse structures have high potential to be applied in sensing, production of new smart materials as well as in medical science.

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“…In order to network stand-alone molecular [10][11][12] or supramolecular [13][14][15][16][17][18][19][20] devices, the functional entities need to be linked by fast chemical communication without harmful interference. All receptors and emitters involved in communication thus need to be highly dynamic and selective with regard to signal uptake, information processing and signal release (= output).…”

mentioning

confidence: 99%