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Rates of Hydroxyl Radical Production from Transition Metals and Quinones in a Surrogate Lung Fluid.

ABSTRACT: Hydroxyl radical ((•)OH) is the most reactive, and perhaps most detrimental to health, of the reactive oxygen species. (•)OH production in lungs following inhalation of particulate matter (PM) can result from redox-active chemicals, including iron and copper, but the relative importance of these species is unknown. This work investigates (•)OH production from iron, copper, and quinones, both individually and in mixtures at atmospherically relevant concentrations. Iron, copper, and three of the four quinones (1,2-naphthoquinone, phenanthrenequinone and 1,4-naphthoquinone) produce (•)OH. Mixtures of copper or quinones with iron synergistically produce (•)OH at a rate 20-130% higher than the sum of the rates of the individual redox-active species. We developed a regression equation from 20 mixtures to predict the rate of (•)OH production from the particle composition. For typical PM compositions, iron and copper account for most (•)OH production, whereas quinones are a minor source, although they can contribute if present at very high concentrations. This work shows that Cu contributes significantly to (•)OH production in ambient PM; other work has shown that Cu appears to be the primary driver of HOOH production and dithiothreitol (DTT) loss in ambient PM extracts. Taken together, these results indicate that copper appears to be the most important individual contributor to direct oxidant production from inhaled PM.

SUBMITTER: Charrier JG

PROVIDER: S-EPMC4777526 | biostudies-literature | 2015 Aug

REPOSITORIES: biostudies-literature

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Rates of Hydroxyl Radical Production from Transition Metals and Quinones in a Surrogate Lung Fluid.

Charrier Jessica G JG Anastasio Cort C

Environmental science & technology 20150720 15

Hydroxyl radical ((•)OH) is the most reactive, and perhaps most detrimental to health, of the reactive oxygen species. (•)OH production in lungs following inhalation of particulate matter (PM) can result from redox-active chemicals, including iron and copper, but the relative importance of these species is unknown. This work investigates (•)OH production from iron, copper, and quinones, both individually and in mixtures at atmospherically relevant concentrations. Iron, copper, and three of the f ...[more]

PMID: 26153923

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Project description:Inhalation of ambient particulate matter causes morbidity and mortality in humans. One hypothesized mechanism of toxicity is the particle-induced formation of reactive oxygen species (ROS) - including the highly damaging hydroxyl radical ((·)OH) - followed by inflammation and a variety of diseases. While past studies have found correlations between ROS formation and a variety of metals, there are no quantitative measurements of (·)OH formation from transition metals at concentrations relevant to 24-hour ambient particulate exposure. This research reports specific and quantitative measurements of (·)OH formation from 10 individual transition metals (and several mixtures) in a cell-free surrogate lung fluid (SLF) with four antioxidants: ascorbate, citrate, glutathione, and uric acid. We find that Fe and Cu can produce (·)OH under all antioxidant conditions as long as ascorbate is present and that mixtures of the two metals synergistically increase (·)OH production. Manganese and vanadium can also produce (·)OH under some conditions, but given that their ambient levels are typically very low, these metals are not likely to chemically produce significant levels of (·)OH in the lung fluid. Cobalt, chromium, nickel, zinc, lead, and cadmium do not produce (·)OH under any of our experimental conditions. The antioxidant composition of our SLF significantly affects (·)OH production from Fe and Cu: ascorbate is required for (·)OH formation, citrate increases (·)OH production from Fe, and both citrate and glutathione suppress (·)OH production from Cu. MINTEQ ligand speciation modeling indicates that citrate and glutathione affect (·)OH production by changing metal speciation, altering the reactivity of the metals. In the most realistic SLF (i.e., with all four antioxidants), Fe generates approximately six times more (·)OH than does the equivalent amount of Cu. Since levels of soluble Fe in PM are typically higher than those of Cu, our results suggest that Fe dominates the chemical generation of (·)OH from deposited particles in the lungs.

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Rates of Hydroxyl Radical Production from Transition Metals and Quinones in a Surrogate Lung Fluid.

Publications

Rates of Hydroxyl Radical Production from Transition Metals and Quinones in a Surrogate Lung Fluid.

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