The prediction of a specific chemical property across a vast library of derivatives represents a formidable challenge. Conventional computational methodologies typically rely on brute-force calculations involving the computation of the property of interest for the entire library or a significant subset. In this study, we present a novel phenomenological approach to address this challenge, employing a perturbation theory-like framework to describe substituent effects.
View Article and Find Full Text PDFThe stereoselective synthesis of geometrical iron(II) complexes bearing azine-NHC ligands is described. Facial and meridional selectivity is achieved as a function of the steric demand of the azine unit, with no remarkable influence of the carbene nature. More specifically, meridional complexes are obtained upon selecting bulky 5-mesityl-substituted pyridyl coordinating units.
View Article and Find Full Text PDFOne major challenge of future sustainable photochemistry is to replace precious and rare transition metals in applications such as energy conversion or electroluminescence by earth-abundant, cheap, and recyclable materials. This involves using coordination complexes of first row transition metals such as Cu, Cr, or Mn. In the case of iron, which is attractive due to its natural abundance, fundamental limitations imposed by the small ligand field splitting energy have recently been overcome.
View Article and Find Full Text PDFTwo novel rhenium(i) tricarbonyl complexes of general formula fac-[Re(N^C:)(CO)X] are herein presented, where N^C: is the pyridoannelated N-heterocyclic carbene (NHC) arising from 2-(2-pyridinyl)imidazo[1,5-a]pyridinium hexafluorophosphate proligand, namely [pyipy]PF, and X being Cl and Br. The synthetic pathway is a one-pot reaction that starts from the azolium salt as the NHC source and [Re(CO)X] to yield the desired charge-neutral fac-[Re(pyipy)(CO)X] complexes (1-2). Both complexes were thoroughly characterized by spectroscopic, electrochemical, theoretical investigation as well as X-ray diffraction analysis.
View Article and Find Full Text PDFObjectives: To assess the prevalence of undiagnosed diabetes and pre-diabetes in the healthy population in the Mollerussa cohort. As a secondary objective, to identify the variables associated with these conditions and to describe the changes in glycaemic status after 1 year of follow-up in subjects with pre-diabetes.
Design: Prospective observational cohort study.