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981.
Dr. Fabio Pirro Dr. Salvatore La Gatta Dr. Federica Arrigoni Dr. Antonino Famulari Dr. Ornella Maglio Prof. Pompea Del Vecchio Prof. Mario Chiesa Prof. Luca De Gioia Prof. Luca Bertini Dr. Marco Chino Prof. Flavia Nastri Prof. Angela Lombardi 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(1):e202211552
De novo metalloprotein design is a remarkable approach to shape protein scaffolds toward specific functions. Here, we report the design and characterization of Due Rame 1 (DR1), a de novo designed protein housing a di-copper site and mimicking the Type 3 (T3) copper-containing polyphenol oxidases (PPOs). To achieve this goal, we hierarchically designed the first and the second di-metal coordination spheres to engineer the di-copper site into a simple four-helix bundle scaffold. Spectroscopic, thermodynamic, and functional characterization revealed that DR1 recapitulates the T3 copper site, supporting different copper redox states, and being active in the O2-dependent oxidation of catechols to o-quinones. Careful design of the residues lining the substrate access site endows DR1 with substrate recognition, as revealed by Hammet analysis and computational studies on substituted catechols. This study represents a premier example in the construction of a functional T3 copper site into a designed four-helix bundle protein. 相似文献
982.
Dr. Fabio Buonsenso Dr. Marta Colombo Dr. Andrea Marchesi Francesca Romana Mammone Prof. Francesco Sannicolò Dr. Roberto Cirilli Prof. Marco Pierini 《European journal of organic chemistry》2023,26(33):e202300568
An experimental and theoretical study was carried out to analyze the configurational lability possessed by some of the most common drugs endowed with a central non-planar seven-membered cycloheptadiene ring, which confers chirality to these compounds. In fact, the absence of planarity allows the existence of two enantiomeric species that can interconvert thanks to a ring overturning mechanism. The energy barrier that opposes the inversion of the chiral tricyclic scaffold characterizing such species, which is strongly dependent on the presence of appropriate substituents on the two external cycles, has been investigated through Dynamic-HPLC and off-column racemization techniques, as well as through assessments based on molecular modelling approaches. Interesting indications were obtained by making targeted structural changes to allow accurate control of the stereolability characterizing the tricyclic framework. 相似文献
983.
Eleonora Colombo Monica Fiorenza Boselli Laura Raimondi Alessandra Puglisi Sergio Rossi 《Helvetica chimica acta》2023,106(10):e202300132
The immobilization of Rose Bengal onto Merrifield resin and its application in the light-driven metal-free thiocyanation of azaheterocycles in continuo were investigated. The supported photocatalyst was used in batch reactions under heterogeneous conditions, with different azaheterocycles, and proved to efficiently promote the reaction. Its recovery and recycle were also demonstrated for up to four times. The resin-supported Rose Bengal was then employed under continuous flow conditions, affording thiocyanate functionalized azaheterocycles with higher space-time-yields than the in-batch transformations, and in a shorter reaction time. The easily modification of the SCN groups was also demonstrated by synthetizing trifluoromethyl thioethers and sulfenyl tetrazoles derivates in high yields. 相似文献
984.
Giancarlo Galli Silvia Gasperetti Massimo Bertolucci Bernard Gallot Federica Chiellini 《Macromolecular rapid communications》2002,23(14):814-818
A new class of fluorinated polymers was prepared by radical ring‐opening homopolymerization of vinylcyclopropane monomers with a perfluorinated (CF2)nF chain (n = 6, 8, or 10). The polymers were in fact copolymers composed of 1,5‐linear and cyclobutane isomer units, the relative content of which depended on n. Surprisingly, they formed liquid‐crystalline mesophases (SmBd and/or SmAd), which was attributed to phase separation of the incompatible fluorocarbon and hydrocarbon components of the repeat unit. 相似文献