Exploiting the catalytic power of enzymes for oxy- and amino-functionalization reactions

Eleonora Grandi

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Biocatalysis might effectively address the challenges associated with green and sustainable chemical synthesis. In the work described in this thesis, native and newly engineered enzymes were used for the step-economic and more sustainable biocatalytic synthesis of valuable precursors to pharmaceuticals and nutraceuticals, including enantioenriched epoxides, vicinal triols and amino acids. First, a non-natural aldolase and a non-natural peroxygenase, both evolved in the laboratory from the promiscuous enzyme 4-oxalocrotonate tautomerase, were combined to develop a one-pot two-step enzymatic cascade for the preparation of α,β-epoxy-aldehydes. The addition of a specifically selected natural epoxide hydrolase to the same pot yielded a short pathway to enantioenriched aryl glycerols from simple biomass-derived starting materials. Second, the laboratory evolution of the enzyme ethylenediamine-N,N'-disuccinic acid (EDDS) lyase generated an enzyme variant that showed a large improvement in activity, enabling the effective and enantioselective synthesis of complex L-aspartic acid derivatives, valuable precursors to the artificial dipeptide sweeteners neotame and advantame. These results present new opportunities to develop practical multienzymatic processes for the more sustainable and step-economic synthesis of an important class of food additives. Finally, a study into the structure, mechanism and biocatalytic potential of a newly discovered monooxygenase, named Rhop3, is presented.
Originele taal-2English
KwalificatieDoctor of Philosophy
Toekennende instantie
  • Rijksuniversiteit Groningen
Begeleider(s)/adviseur
  • Poelarends, Gerrit, Supervisor
  • Thunnissen, Andy, Co-supervisor
Datum van toekenning20-jun.-2023
Plaats van publicatie[Groningen]
Uitgever
DOI's
StatusPublished - 2023

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