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Enzyme-Mediated Dynamic Combinatorial Chemistry

Descrizione del progetto

Usare i modelli per guidare la sintesi enzimatica

In natura, i modelli biomolecolari definiscono i risultati delle reazioni enzimatiche in alcuni dei processi biologici più fondamentali, come la replicazione del DNA, la trascrizione e la traduzione. Il progetto ENZYME-DCC, finanziato dall’UE, approfondirà la possibilità di utilizzare modelli sintetici (artificiali) per guidare le reazioni enzimatiche e accedere a prodotti diversi da quelli formati in natura. I ricercatori esamineranno un approccio concettualmente nuovo all’uso degli enzimi per la sintesi chimica, che prevede la combinazione di strumenti e concetti della chimica sintetica con l’enzimologia. In questa nuova metodologia, gli enzimi catalizzano reazioni reversibili e generano complesse miscele dinamiche di prodotti interconvertiti. Si aggiungono quindi molecole modello artificiali per riconoscere e selezionare i prodotti desiderati dalle miscele.

Obiettivo

Biomolecular templates define the outcomes of enzymatic reactions in some of the most fundamental of biological processes, such as DNA replication, transcription and translation. In synthetic chemistry, molecular templates have enabled the synthesis of highly complex molecular architectures and interlocked structures. The possibility to use synthetic templates to direct enzymatic reactions and obtain alternative products to those generated in Nature will be investigated in this project. The overall objective of this research programme is to explore a conceptually new approach to the use of enzymes for chemical synthesis and thus establish a new synthetic methodology - Template-Directed Enzyme-Mediated Dynamic Combinatorial Chemistry. We will exploit the inherent reversibility of enzymatic reactions to generate dynamic chemical networks, which can be manipulated via supramolecular interactions with artificial template molecules to promote the preferential synthesis of specific products. To implement this novel concept, we will develop an unprecedented, templated, enzymatic approach to oligosaccharide synthesis. We will explore dynamic systems of interconverting glycans with the goal of accessing unusual or challenging oligosaccharide products. The specific aims are: 1. To achieve templated enzymatic selective synthesis of large-ring cyclodextrins (cyclodextrins (CDs) with more than 8 glucose units). 2. To explore cyclodextrin glucanotransferase-mediated dynamic mixtures of modified CDs, and, using thiol-functionalised CDs, develop a doubly dynamic system that combines reversible transglycosylation with disulfide exchange. 3. To generate phosphorylase-mediated dynamic mixtures of linear α-1,4-glycans and employ templates to achieve length- and sequence-selective synthesis. 4. To establish a fuelled far-from-equilibrium system for continuous large-ring CD synthesis using templates together with a series of interconnected dynamic enzymatic transformations.

Istituzione ospitante

DANMARKS TEKNISKE UNIVERSITET
Contribution nette de l'UE
€ 1 499 993,00
Indirizzo
ANKER ENGELUNDS VEJ 101
2800 Kongens Lyngby
Danimarca

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Regione
Danmark Hovedstaden Københavns omegn
Tipo di attività
Higher or Secondary Education Establishments
Collegamenti
Costo totale
€ 1 499 997,00

Beneficiari (1)