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Electrochemical and spectroelectrochemical investigation of Ru(por)(NO)(OAr) derivatives (por = octaethylporphyrin, tetraanisolylporphyrin; Ar = Ph, CH-2-NHC(O)CF; CH-2,6-(NHC(O)CF)).
Dalton Trans
January 2025
Department of Chemistry, Southern Illinois University Edwardsville, Edwardsville, IL, 62025-1652 USA.
The electrochemistry and spectroelectrochemistry of Ru(porphyrin)(NO)(phenoxide) complexes Ru(por)(NO)(OPh) (por = OEP, 1a; TAP, 2a; Ph = CH), Ru(por)(NO)(OAr) (por = OEP, 1b; TAP, 2b; OAr = -OCH-(2-NHC(O)CF)), Ru(por)(NO)(OAr) (por = OEP, 1c; TAP, 2c; OAr = OCH-(2,6-NHC(O)CF); OEP = octaethylporphyrinato dianion, TAP = tetraanisolylporphyrinato dianion) indicate that initial one-electron oxidation results in structure-dependent net reactivity at the phenoxide ligand. Oxidation of 1a generates 1a+, which undergoes a relatively slow rate-limiting second-order follow-up reaction. In contrast, 2a undergoes a diffusion-limited follow-up reaction after oxidation.
View Article and Find Full Text PDFModulation of Molecular Quadrupole Moments by Phenyl Side-Chain Fluorination for High-Voltage and High-Performance Organic Solar Cells.
J Am Chem Soc
January 2025
College of Biological, Chemical Sciences and Engineering, Jiaxing University, Jiaxing 314001, China.
The ground-state charge generation (GSCG) in photoactive layers determines whether the photogenerated carriers occupy the deep trap energy levels, which, in turn, affects the device performance of organic solar cells (OSCs). In this work, charge-quadrupole electrostatic interactions are modulated to achieve GSCG through a molecular strategy of introducing different numbers of F atom substitutions on the BTA3 side chain. The results show that 8F substitution (BTA3-8F) and 16F substitution (BTA3-16F) lead to different patterns of highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy level changes.
View Article and Find Full Text PDFStructure, kinetics, and mechanism of Pseudomonas putida sulfoquinovose dehydrogenase, the first enzyme in the sulfoglycolytic Entner-Doudoroff pathway.
Biochem J
January 2025
School of Chemistry and Bio21 Molecular Science and Biotechnology Institute, University of Melbourne, Parkville, Victoria 3010, Australia.
The sulfosugar sulfoquinovose (SQ) is catabolized through the sulfoglycolytic Entner-Doudoroff pathway, beginning with the oxidation of SQ to sulfogluconolactone by SQ dehydrogenase. We present a comprehensive structural and kinetic characterization of Pseudomonas putida SQ dehydrogenase (PpSQDH). PpSQDH is a tetrameric enzyme belonging to the short-chain dehydrogenase/reductase (SDR) superfamily with a strong preference for NAD+ over NADP+.
View Article and Find Full Text PDFCitrullination at the N-terminal region of MDM2 by the PADI4 enzyme.
Protein Sci
February 2025
Instituto de Biocomputación y Física de Sistemas Complejos (BIFI), Universidad de Zaragoza, Zaragoza, Spain.
PADI4 is one of the human isoforms of a family of enzymes involved in the conversion of arginine to citrulline. MDM2 is an E3 ubiquitin ligase that is critical for degradation of the tumor suppressor gene p53. We have previously shown that there is an interaction between MDM2 and PADI4 in cellulo, and that such interaction occurs through the N-terminal region of MDM2, N-MDM2, and in particular through residues Thr26, Val28, Phe91, and Lys98.
View Article and Find Full Text PDFLow-energy electron driven reactions in 2-bromo-5-nitrothiazole.
J Chem Phys
January 2025
Institut für Ionenphysik und Angewandte Physik, Universität Innsbruck, Technikerstraße 25, A-6020 Innsbruck, Austria.
Thiazole derivatives are biologically relevant molecules, used also in pharmaceutical applications. Herein, we report results for electron attachment to 2-bromo-5-nitrothiazole (BNT) in the gas phase. Employing two crossed electron-molecule beam experiments, we determined the efficiency curves of various fragment anions as a function of the initial electron energy between about 0 and 10 eV as well as the emission angle and kinetic energy distributions of Br- and NO2- ions formed from a resonance near 4 eV.
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