Hydroxyl radical generation by electron paramagnetic resonance as a new method to monitor ambient particulate matter composition

Shi, Tingming; Schins, Roel P. F.; Knaapen, Ad M.; Kuhlbusch, Thomas A. J.; Pitz, Mike; Heinrich, Joachim; Borm, Paul

doi:10.1039/b303928p

Cited by 184 publications

(132 citation statements)

References 32 publications

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“…These data show the importance of secondary atmospheric processes to OP WI-DTT . The results are consistent with studies that have found water-insoluble DTTactive constituents could be secondary quinones from oxidized polycyclic aromatic hydrocarbons that remain bound to the surface of soot particles associated with traffic emissions (Antinolo et al, 2015;Li et al, 2013;Shiraiwa et al, 2012). This means that, although roadway emissions are a source for components that contribute to OP, some form of processing is needed to convert the roadway emissions to species with measurable oxidative potential for both OP Total-DTT and OP WS-DTT .…”

Section: Op Ws-dtt and Op Total-dtt Measurements On Quartz Versus Tefsupporting

confidence: 80%

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A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP

et al. 2017

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Abstract. An automated analytical system was developed for measuring the oxidative potential (OP) with the dithiothreitol (DTT) assay of filter extracts that include both watersoluble and water-insoluble (solid) aerosol species. Three approaches for measuring total oxidative potential were compared. These include using methanol as the solvent with (1) and without (2) filtering the extract, followed by removing the solvent and reconstituting with water, and (3) extraction in pure water and performing the OP analysis in the extraction vial with the filter. The water extraction method (the third approach, with filter remaining in the vial) generally yielded the highest DTT responses with better precision (coefficient of variation of 1-5 %) and was correlated with a greater number of other aerosol components. Because no organic solvents were used, which must be mostly eliminated prior to DTT analysis, it was easiest to automate by modifying an automated analytical system for measuring water-soluble OP developed by . Therefore, the third method was applied to the field study for the determination of total OP. Daily 23 h filter samples were collected simultaneously at a roadside (RS) and a representative urban (Georgia Tech, GT) site for two 1-month study periods, and both water-soluble (OP WS-DTT ) and total (OP Total-DTT ) OP were measured. Using PM 2.5 (aerodynamic diameter < 2.5 µm) high-volume samplers with quartz filters, the OP WS-DTT -to-OP Total-DTT ratio at the urban site was 65 % with a correlation coefficient (r) of 0.71 (N = 35; p value < 0.01), compared to a ratio of 62 % and r = 0.56 (N = 31; p value < 0.01) at the roadside site. The same DTT analyses were performed, and similar results were found using particle composition monitors (flow rate of 16.7 L min −1 ) with Teflon filters. Comparison of measurements between sites showed only slightly higher levels of both OP WS-DTT and OP Total-DTT at the RS site, indicating both OP WS-DTT and OP Total-DTT were largely spatially homogeneous. These results are consistent with roadway emissions as sources of DTT-quantified PM 2.5 OP and indicate that both soluble and insoluble aerosol components contributing to OP are largely secondary.

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Section: Op Ws-dtt and Op Total-dtt Measurements On Quartz Versus Tefsupporting

confidence: 80%

“…Various methods have been developed to assess PM OP (Ayres et al, 2008;Cho et al, 2005;King and Weber, 2013;Mudway et al, 2004;Shi et al, 2003;Wang et al, 2011). The dithiothreitol (DTT) assay is used in this study to measure the OP of fine particles (i.e., OP DTT ).…”

Section: Introductionmentioning

confidence: 99%

A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP

et al. 2017

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“…Fe is often linked to the oxidative damage caused by particles (Valavanidis et al, 2000;Han et al, 2001;See et al, 2007;Di Pietro et al, 2009;Charrier and Anastasio, 2011), and soluble Fe affects oxidative capacity through (Shi et al, 2003;Risom et al, 2005;Vidrio et al, 2008;Nawrot et al, 2009). The ICP-MS analysis indicated that, although total Fe concentration in the Lanzhou PM 10 samples was much higher than that in the soluble fraction, the concentration of soluble Fe was significant, reaching as much as 1105 μg/g.…”

Section: Correlation Between Heavy Metal Concentration and Bioreactivitymentioning

confidence: 98%

Heavy Metal Compositions and Bioreactivity of Airborne PM10 in a Valley-Shaped City in Northwestern China

Xiao

Shao

Zhang³

et al. 2013

Aerosol Air Qual. Res.

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Lanzhou, a valley-shaped city in northwestern China, experiences heavy air pollution. This study investigated the relationship between the oxidative capacity and heavy metal composition of the PM 10 in Lanzhou. Inductively coupled plasma-mass spectrometry (ICP-MS) was used to examine the heavy metal element composition and an in vitro plasmid assay was employed to study the bioreactivity of airborne PM 10 . The monitoring data revealed that the mass concentration of Lanzhou PM 10 exhibited seasonal variations at both the urban and suburban sites, with higher values in winter and spring, lower values in autumn, and the lowest ones in summer. The results of ICP-MS analysis showed that Zn was the metal present in the highest concentrations in both the whole and water-soluble fractions of PM 10 collected at both the urban and suburban sites, followed by Fe, Pb, and Mn. Furthermore, the results indicated that Zn, Cd, and As were present mostly in their soluble forms, while the Fe, Pb, and V were primarily in their insoluble ones. The plasmid DNA assay results indicated that the TD 20 values (toxic dosages of PM 10 causing 20% of plasmid DNA damage) of the Lanzhou PM 10 collected at both the urban and suburban sites ranged from 10 μg/mL to over 1000 μg/mL, and exhibited seasonal variations. The TD 20 values were high in spring and autumn, and thus the toxicities were low, while the TD 20 values were low in winter and summer, and thus the toxicities were high. For PM 10 collected at both the urban and suburban sites, the high concentrations of water-soluble Zn, Fe, Pb, and Mn displayed a strong negative correlation with the TD 20 values, suggesting that these metals were likely the major elements responsible for plasmid DNA damage. In addition, meteorological conditions (i.e., lower wind speed and higher relative humidity) during the sampling periods may have caused an indirect increase in oxidative damage to DNA.

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“…DTT is known to react with organic compounds but also with transition metals (Charrier and Anastasio, 2012;Lin and Yu, 2011). The ESR assay employs the spin trap 5,5-Dimethyl-1-pyrroline N-oxide (DMPO) and is specific for reactive radical species, which for example result from partial reduction of dioxygen catalyzed by transition metal (Boogaard et al, 2012;Shi et al, 2003). The AA assays would be more 30 specific to the oxidative potential of transition metals (Godri et al, 2011;, but ascorbic acid is known to react with organics such as quinones (Shang et al, 2012;Visentin et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

Comparison between five acellular oxidative potential measurement assays performed with detailed chemistry on PM<sub>10</sub> samples from the city of Chamonix (France)

Calas¹,

Uzu²,

Kelly³

et al. 2017

Preprint

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Abstract. Many studies have demonstrated associations between exposure to ambient particulate matter (PM) and adverse health outcomes in humans that can be explained by PM capacity to induce oxidative stress in vivo. Thus, assays have been developed to quantify the oxidative potential (OP) of PM as a more refined exposure metric than PM mass alone. Only a 15 small number of studies have compared different acellular OP measurements for a given set of ambient PM samples. Yet, fewer studies have compared different assays over a year long period and with detailed chemical characterization of ambient PM. In this study, we report on seasonal variations of the dithiothreitol (DTT), ascorbic acid (AA), electron spin resonance (ESR) and the respiratory tract lining fluid (RTLF, composed of the reduced glutathione (GSH) and ascorbic acid (ASC)) assays over a one year period in which 100 samples were analysed. A detailed PM 10 characterization allowed univariate and 20 multivariate regression analyses in order to obtain further insight into groups of chemical species that drive OP measurements. Our results show that most of the OP assays were strongly inter-correlated over the sampling year but also these correlations differed when considering specific sampling periods (cold vs warm). All acellular assays are correlated with a significant number of chemical species when considering univariate correlations, especially for the DTT assay.Evidence is also presented of a seasonal contrast over the sampling period with significantly higher OP values during winter 25 for the DTT, AA, GSH and ASC assays, which were assigned to biomass burning species by the multiple linear regression models. The ESR assay clearly differs from the other tests as it did not show seasonal dynamics and presented weaker correlations with other assays and chemical species.Atmos. Chem. Phys. Discuss., https://doi

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Hydroxyl radical generation by electron paramagnetic resonance as a new method to monitor ambient particulate matter composition

Cited by 184 publications

References 32 publications

A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP

A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP

Heavy Metal Compositions and Bioreactivity of Airborne PM10 in a Valley-Shaped City in Northwestern China

Comparison between five acellular oxidative potential measurement assays performed with detailed chemistry on PM<sub>10</sub> samples from the city of Chamonix (France)

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Hydroxyl radical generation by electron paramagnetic resonance as a new method to monitor ambient particulate matter composition

Cited by 184 publications

References 32 publications

A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP

A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP

Heavy Metal Compositions and Bioreactivity of Airborne PM10 in a Valley-Shaped City in Northwestern China

Comparison between five acellular oxidative potential measurement assays performed with detailed chemistry on PM&lt;sub&gt;10&lt;/sub&gt; samples from the city of Chamonix (France)

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Comparison between five acellular oxidative potential measurement assays performed with detailed chemistry on PM<sub>10</sub> samples from the city of Chamonix (France)