Methods for regioselective N-methylation and -alkylation of unsaturated heterocycles with “off the shelf” reagents are highly sought-after. This reaction could drastically simplify synthesis of privileged bioactive molecules. Here we report engineered and natural methyltransferases for challenging N-(m)ethylation of heterocycles, including benzimidazoles, benzotriazoles, imidazoles and indazoles. The reactions are performed through a cyclic enzyme cascade that consists of
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In this research article, we describe a 4H+/4e– electron-coupled-proton buffer (ECPB) based on Cu and a redox-active ligand. The protonated/reduced ECPB (complex 1: [Cu(8H+/14e–)]1+), consisting of CuI with 2 equiv of the ligand (catLH4: 1,1?-(4,5-dimethoxy-1,2-phenylene)bis(3-(tert-butyl)urea)), reacted with H+/e– acceptors such as O2 to generate the deprotonated/oxidized ECPB. The resulting compound, (complex 5: [Cu(4H+/10e–)]1+), was characterized
The aerobic oxidation of alkenes to carbonyls is an important and challenging transformation in synthesis. Recently, a new P450-based enzyme (aMOx) has been evolved in the laboratory to directly oxidize styrenes to their corresponding aldehydes with high activity and selectivity. The enzyme utilizes a heme-based, high-valent iron-oxo species as a catalytic oxidant that normally epoxidizes
Last week (Aug 28th to Sept 2nd 2022) took place the 19th International Conference on Density Functional Theory and its Applications in Burssels, which included a poster session. Gerard Comas, PhD student under the supervision of Dr. Pedro Salvador, presented a poster titled “Accurate 57Fe Mössbauer Parameters from General Gaussian Basis sets”, and won one
In this work, we propose specific electrolyte formulations for Na-ion batteries comprising linear and cyclic ether-based solvents and sodium trifluoromethanesulfonate salt that are thermally stable down to ?150?°C and enable the formation of stable solid electrolyte interphase at low temperatures. It shows the excellent performance of Na-ion batteries at very low temperatures, essential for their
During this week (Sep 4-7) there will be the second main event of the year: #ADHOC2022 at the “La Mercè” Auditorium organised by Bioinspired, Supramolecular and Catalysis Chemistry group (QBIS-CAT) of the Institute of Computational Chemistry and Catalysis (IQCC) from University of Girona. The International Symposium on Activation of Dioxygen and Homogeneous Oxidation Catalysis (ADHOC 2022) is a
Recently, Daniel Bosch, Jun Wang and Lluís Blancafort reported in Chemical Science on “Fingerprint-based deep neural networks can model thermodynamic and optical properties of eumelanin DHI dimers”. Eumelanin is the biopolymer responsible for photoprotection in living beings and holds great promise as a smart biomaterial, but its detailed structure has not been characterized experimentally. Theoretical models
This week, our member of IQCC Margarida Borrell was awarded the annual recognition of the best PhD thesis in 2021 (Premi Extraordinari) from the University of Girona. Last year, he defended with success her PhD thesis on “Small-molecule mimics of Rieske oxygenases. Application to selective aliphatic C-H hydroxylation and olefin syn-dihydroxylation”, supervised by Miquel Costas.
Oxidant-free Au-catalyzed reactions are emerging as a new synthetic tool for innovative organic transformations. Still, a deeper mechanistic understanding is needed for a rational design of these processes. Here we describe the synthesis of two Au(I) complexes bearing bidentated hemilabile MICˆN ligands, [AuI(MICˆN)Cl], and their ability to stabilize square-planar Au(III) species (MIC = mesoionic carbene).