A5061723798- Asymmetric Hydrogenation and Catalysis
- Chemical Synthesis and Analysis
- Cyclopropane Reaction Mechanisms
- Nanomaterials for catalytic reactions
- Click Chemistry and Applications
- Peptidase Inhibition and Analysis
- Advanced Polymer Synthesis and Characterization
- Metalloenzymes and iron-sulfur proteins
- Surface Chemistry and Catalysis
- Organometallic Complex Synthesis and Catalysis
- Ferrocene Chemistry and Applications
- Chemical Reactions and Isotopes
- Synthesis of β-Lactam Compounds
- biodegradable polymer synthesis and properties
- Synthesis and Catalytic Reactions
- Enzyme Catalysis and Immobilization
- Mosquito-borne diseases and control
- Nanocluster Synthesis and Applications
- Radical Photochemical Reactions
- Porphyrin and Phthalocyanine Chemistry
- Cancer Treatment and Pharmacology
- Biochemical and Structural Characterization
- Catalytic C–H Functionalization Methods
- Electrochemical sensors and biosensors
- Malaria Research and Control
Adolphe Merkle Institute
2018-2022
University of Fribourg
2018-2022
University of Basel
2015-2022
Fribourg Development Agency
2020
Webb Institute
2020
University of Milan
2011-2015
Mylan (South Africa)
2015
An E. coli platform for systematic engineering of artificial metalloenzymes that catalyze new-to-nature reactions is described.
Artifical metalloenzymes combine the reactivity of small molecule catalysts with selectivity enzymes, and new methods are required to tune catalytic properties these systems for an application interest. Structure-based computational design could help identify amino acid mutations leading improved activity enantioselectivity. Here we describe Rosetta Design genetic optimization artificial transfer hydrogenase (ATHase hereafter), [(η5-Cp*)Ir(pico)Cl] ⊂ WT hCA II (Cp* = Me5C5–), asymmetric...
Artificial metalloenzymes (ArMs), which combine an abiotic metal cofactor with a protein scaffold, catalyze various synthetically useful transformations. To complement the natural enzymes' repertoire, effective optimization protocols to improve ArM's performance are required. Here we report on our efforts optimize activity of artificial transfer hydrogenase (ATHase) using Escherichia coli whole cells. For this purpose, rely self-immolative quinolinium substrate which, upon reduction,...
Reversible-deactivation radical polymerizations (controlled polymerizations) have revolutionized and revitalized the field of polymer synthesis. While enzymes other biologically derived catalysts long been known to initiate free polymerizations, ability peroxidases, hemoglobin, laccases, enzyme-mimetics, chlorophylls, heme, red blood cells, bacteria, biocatalysts control or reversible-deactivation has only described recently. Here, scope biocatalytic atom transfer (bioATRP), enzyme-initiated...
The streptavidin scaffold was expanded with well-structured naturally occurring motifs. These chimeric scaffolds were tested as hosts for biotinylated catalysts artificial metalloenzymes (ArM) asymmetric transfer hydrogenation, ring-closing metathesis and anion−π catalysis. additional second coordination sphere elements significantly influence both the activity selectivity of resulting hybrid catalysts. findings lead to identification propitious streptavidins future directed evolution...
Abstract The possibility of obtaining an efficient artificial imine reductase was investigated by introducing a chiral cofactor into metalloenzymes based on biotin–streptavidin technology. In particular, biotinylated 1,3‐diamine ligand in coordination with iridium(III) complex developed. Optimized chemogenetic studies afforded positive results the stereoselective reduction cyclic imine, salsolidine precursor, as standard substrate access to both enantiomers. Various factors such pH,...
A new efficient synthesis of 1,3-diamines was realized and their ruthenium(<sc>ii</sc>) complexes were studied in ATH aqueous media.
Myoglobin was subjected to site-directed mutagenesis and transformed into a catalyst able perform atom transfer radical cyclisation reactions,
Abstract Ruthenium(II) dichlorides with racemic atropos‐biaryl‐based diphosphanes and optically active 1,2‐diphenylethane‐1,2‐diamine (DPEN) as ligands have been synthesised. trans cis isomers were formed due to the low basicity of diphosphane ligands, in particular, BITIANP BIMIP. The species easily separated by filtration. In when rac ‐BITIANP was used combination chiral DPEN, asymmetric separation pure complexes arrangements realised they precatalysts hydrogenation ketones. Matching...
Chiral (R)-(-) and (S)-(+)-8-amino-5,6,7,8-tetrahydroquinoline, hereafter defined (R)-CAMPY (S)-CAMPY, have proved to be valuable chiral ligands in Ru(II) precatalysts for the reduction of prochiral ketones by asymmetric hydrogen transfer AHT. These bear information on an alkyl ring fused a pyridine therefore flat nature, characterized high conformational rigidity. It represent first application AHT member family ancillary already known as starting material medicinal compouds. The reaction...
Abstract Myoglobin (Mb) can react with hydrogen peroxide (H 2 O ) to form a highly active intermediate compound and catalyse oxidation reactions. To enhance this activity, known as pseudo‐peroxidase previous studies have focused on the modification of key amino acid residues Mb or heme cofactor. In work, scaffold (apo‐Mb) was systematically reconstituted set cofactors based six metal ions two ligands. These variants were fully characterised by UV‐Vis spectroscopy, circular dichroism (CD)...
A highly sensitive polymerization assay to detect the malaria biomarker hemozoin was accelerated less than 4 minutes.
Abstract Artificial metalloenzymes (ArMs) catalyzing new-to-nature reactions under mild conditions could play an important role in the transition to a sustainable, circular economy. While ArMs have been created for variety of bioorthogonal transformations, attempts at optimizing their performance by enzyme engineering case-specific and resulted only modest improvements. To realize full potential ArMs, methods that enable rapid discovery highly active ArM variants any reaction interest are...