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Intervalence Charge Transfer in an Osmium(IV) Tetra(ferrocenylaryl) Complex.
Inorg Chem
January 2025
Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States.
The functional properties of tetraaryl compounds, M(aryl) (M = transition metal or group 14 element), are dictated not only by their common tetrahedral geometry but also by their central atom. The identity of this atom may serve to modulate the reactivity, electrochemical, magnetic, and optical behavior of the molecular species, or of extended materials built from appropriate tetraaryl building blocks, but this has not yet been systematically evaluated. Toward this goal, here we probe the influence of Os(IV), C, and Si central atoms on the spectroelectrochemical properties of a series of redox-active tetra(ferrocenylaryl) complexes.
View Article and Find Full Text PDFFacile Access to Terminal Nitroalkanes via Anti-Markovnikov Hydronitration and Hydronitroalkylation of Alkenes Using Photoredox Catalysis.
Chemistry
December 2024
Department of Chemistry, Biochemistry, and Pharmaceutical Sciences, University of Bern (UniBe), Freiestrasse 3, 3012, Bern, Switzerland.
The evolution of catalysis and functional group transfer reagents play a significant role in the development of anti-Markovnikov alkene hydrofunctionalization reactions, facilitating the access to value-added molecules. We herein report the first rational design of a modular intermolecular anti-Markovnikov hydronitration of alkenes, enabling the direct synthesis of terminal nitroalkanes under visible light-mediated photoredox catalysis. By employing the redox-active organic nitrating reagent N-nitrosuccinimide, the produced nitryl radicals, in the presence of an olefin and a hydrogen atom transfer (HAT) mediator, lead to an anti-Markovnikov addition with complete regioselectivity.
View Article and Find Full Text PDFFluorescence-Based Proteoliposome Methods to Monitor Redox-Active Transition Metal Transmembrane Translocation by Metal Transporters.
Methods Mol Biol
July 2024
Department of Chemistry and Biochemistry, The University of Texas at Dallas, Richardson, TX, USA.
Transmembrane transition metal transporter proteins are central gatekeepers in selectively controlling vectorial metal cargo uptake and extrusion across cellular membranes in all living organisms, thus playing key roles in essential and toxic metal homeostasis. Biochemical characterization of transporter-mediated translocation events and transport kinetics of redox-active metals, such as iron and copper, is challenged by the complexity in generating reconstituted systems in which vectorial metal transport can be studied in real time. We present fluorescence-based proteoliposome methods to monitor redox-active metal transmembrane translocation upon reconstitution of purified metal transporters in artificial lipid bilayers.
View Article and Find Full Text PDFDevelopment of Modular Nitrenium Bipolar Electrolytes for Possible Applications in Symmetric Redox Flow Batteries.
J Am Chem Soc
July 2024
Department of Chemistry, University of Utah, Salt Lake City, Utah 84112, United States.
Amid the escalating integration of renewable energy sources, the demand for grid energy storage solutions, including non-aqueous organic redox flow batteries (oRFBs), has become ever more pronounced. oRFBs face a primary challenge of irreversible capacity loss attributed to the crossover of redox-active materials between half-cells. A possible solution for the crossover challenge involves utilization of bipolar electrolytes that act as both the catholyte and anolyte.
View Article and Find Full Text PDFEffect of Hydrodynamic Interactions and Flow on Charge Transport in Redox-Active Polymer Solutions.
J Phys Chem B
February 2024
Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
Redox-active polymers (RAPs) are a subclass of polyelectrolytes that can store charge and undergo redox self-exchange reactions. RAPs are of great interest in the field of redox flow batteries (RFBs) due to their ability to quickly charge and discharge, their chemical modularity, and their molecular size. However, designing RAPs for efficient charge transport at the molecular level requires a fundamental understanding of the charge transport mechanisms that occur in RFBs.
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