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Catalytic radical reduction in aqueous solution via oxidation of biologically-relevant alcohols.

ABSTRACT: Metalloenzymes that normally perform catalytic antioxidant or radical-degrading functions, as well as small-molecule complexes that mimic them, can also exert pro-oxidant or radical-forming effects depending on the identity of the terminal reductant. Because nitroxyl radicals function as redox active cocatalysts in the aerobic oxidation of alcohols, we hypothesized that catalytic radical reduction could be achieved via the oxidation of biologically-relevant alcohols. Herein we report an organoruthenium complex (Ru1) that catalyzed reduction of 2,2'-azino-bis(3-ethylbenzo-thiazoline-6-sulfonate) radical monoanion (ABTS˙^-) to ABTS^2- in phosphate buffered saline (pH 7.4) using MeOH, EtOH, i-PrOH, serine, threonine, glucose, arabinose, methyl lactate or dimethyl malate as the terminal reductant. Replacing either the C-H or O-H groups of a -CHOH- moiety resulted in the loss of ABTS˙^- reducing ability. Moreover, in conjunction with an alcohol terminal reductant, Ru1 was able to inhibit the oxidation of ABTS^2- by H₂O₂ and horseradish peroxidase, even after multiple successive challenges with excess H₂O₂ or ABTS˙^-. Collectively, these results demonstrate that Ru1 inhibits the oxidative formation of and catalyzes the reduction of radicals in aqueous solution via oxidation of biologically-relevant alcohols.

SUBMITTER: Htet Y

PROVIDER: S-EPMC6013915 | biostudies-literature | 2016 Jul

REPOSITORIES: biostudies-literature

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Catalytic radical reduction in aqueous solution <i>via</i> oxidation of biologically-relevant alcohols.

Htet Yamin Y Tennyson Andrew G AG

Chemical science 20160310 7

Metalloenzymes that normally perform catalytic antioxidant or radical-degrading functions, as well as small-molecule complexes that mimic them, can also exert pro-oxidant or radical-forming effects depending on the identity of the terminal reductant. Because nitroxyl radicals function as redox active cocatalysts in the aerobic oxidation of alcohols, we hypothesized that catalytic radical reduction could be achieved <i>via</i> the oxidation of biologically-relevant alcohols. Herein we report an o ...[more]

PMID: 30155048

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Project description:The synthesis of optoelectrically enhanced nanomaterials should be continuously improved by employing time- and energy-saving techniques. The porous zinc oxide (ZnO) and copper-doped ZnO nanocomposites (NCs) were synthesized by the time- and energy-efficient solution combustion synthesis (SCS) approach. In this SCS approach, once the precursor-surfactant complex ignition point is reached, the reaction starts and ends within a short time without the need for any external energy. The TGA-DTA analysis confirmed that 500 °C was the point at which stable metal oxide was obtained. The doping and heterojunction strategy improved the optoelectric properties of the NCs more than the individual constituents, which then enhanced the materials' charge transfer and optical absorption capabilities. The porosity, nanoscale crystallite size (15-50 nm), and formation of Cu/CuO-ZnO NCs materials were confirmed from the XRD, SEM, and TEM/HRTEM analyses. The obtained d-spacing values of 0.275 and 0.234 nm confirm the formation of ZnO and CuO crystals, respectively. The decrease in photoluminescence intensity for the doped NCs corroborates a reduction in electron-hole recombination. On the Mott-Schottky analysis, the positive slope for ZnO confirms the n-type character, while the negative and positive slopes of the NCs confirm the p- and n-type characters, respectively. A diffusion-controlled type of charge transfer process on the electrode surface was confirmed from the cyclic voltammetric analysis. Thus, the overall analysis shows the applicability of the less expensive and more efficient SCS for several applications, such as catalysis and sensors. To confirm this, an organic catalytic reduction reaction of 4-nitrophenol to 4-aminophenol was tested. Within three and a half minutes, the catalytic reduction result showed the great potential of NCs over ZnO NPs. Thus, the energy- and time-saving SCS approach has a great future outlook as an industrial pollutant catalytic reduction application.

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Catalytic radical reduction in aqueous solution via oxidation of biologically-relevant alcohols.

Publications

Catalytic radical reduction in aqueous solution <i>via</i> oxidation of biologically-relevant alcohols.

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