A characterization of HULIS-C and the oxidative potential of HULIS and HULIS-Fe(II) mixture in PM2.5 during hazy and non-hazy days in Shanghai

Lü, Sihua; Win, Myat Sandar; Zeng, Junyang; Yao, Chuanhe; Zhao, Mengfei; Xiu, Guangli; Lin, Yu‐Hsuan; Xie, Tingting; Dai, Yafeng; Rao, Lanfang; Zhang, Luying; Yonemochi, Shinich; Wang, Qingyue

doi:10.1016/j.atmosenv.2019.117058

Cited by 28 publications

(10 citation statements)

References 40 publications

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“…(1) WSOC could synergistically interact with Fe to enhance its macrophage ROS activity, and (2) WSOC enhances the solubility of Fe through complexation, making it available for macrophage ROS generation. Although there are studies showing the interaction of Fe with HULIS in the acellular 34−36 and cellular assays, 37,38 the results shown in Figure 2, i.e., the close agreement of the sum of the OPs from hydrophobic and hydrophilic fractions with the total activity of the original PM 2.5 water-soluble extract, do not support that.…”

Section: ■ Results and Discussionmentioning

confidence: 89%

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM_2.5

Wang

Salana

et al. 2022

Environ. Sci. Technol. Lett.

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Previous studies have indicated the roles of both organic compounds and metals in driving the cellular generation of reactive oxygen species (ROS); however, their contribution has not been adequately quantified using mechanistic approaches. We developed a novel fractionation scheme for the stepwise removal of various classes of organic compounds and metals using a combination of solid phase extraction columns. We applied this fractionation scheme to 10 PM 2.5 samples collected from the midwestern United States. Because both watersoluble organic carbon (WSOC) and Fe have shown good correlations with cellular ROS, we separated them into different fractions and measured their ability to generate ROS in rat alveolar macrophages. Most of the PM 2.5 cellular ROS was attributed to the metallic fraction. To further explore the reason for the correlation of WSOC with ROS, we investigated the water solubility of Fe by measuring the total Fe in PM 2.5 samples. The water-soluble fraction of Fe was tightly correlated with WSOC (r ≥ 0.69), indicating WSOC may have an additional role in cellular oxidative potential, probably through complexation of Fe, in enhancing its water solubility and macrophage ROS activity. This work reveals the role of both Fe and organic compounds through different mechanisms in contributing to PM 2.5 -driven cellular ROS.

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Section: ■ Results and Discussionmentioning

confidence: 89%

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM_2.5

Wang

Salana

et al. 2022

Environ. Sci. Technol. Lett.

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“…HULIS alone showed a stronger oxidative potential than the HULIS-Fe 3+ complexation. Incredibly, HULIS exhibited high free-cell mortality affected by ROS when reacting with the Fe ion solution for 40 min, implying that the oxidative activity of HULIS was affected by the complexation time with the metal ions . The absorbance of atmospheric HULIS did not change significantly from 0 to 30 min after the action of Cu 2+ , Zn 2+ , and Al 3+ ions, and 1 O 2 and · OH expressed significant EPR signals only after 30 min of light irradiation.…”

Section: Resultsmentioning

confidence: 94%

“…Incredibly, HULIS exhibited high free-cell mortality affected by ROS when reacting with the Fe ion solution for 40 min, implying that the oxidative activity of HULIS was affected by the complexation time with the metal ions. 84 The absorbance of atmospheric HULIS did not change significantly from 0 to 30 min after the action of Cu 2+ , Zn 2+ , and Al 3+ ions, and 1 O 2 and • OH expressed significant EPR signals only after 30 min of light irradiation. Considering the complete coupling between metals and atmospheric HULIS and the large formation of ROS, 30 min was chosen as the reaction time between metal ions and atmospheric HULIS, which was in good agreement with the study of Wan et al 68 Atmospheric HULIS was affected by the coupling of four metal ions, which promoted its photochemical production of • OH and 1 O 2 to varying degrees.…”

Section: Effect Of Ros Generation Of Atmospheric Hulis Under Metal Io...mentioning

confidence: 85%

Significant Promotion of Light Absorption Ability and Formation of Triplet Organics and Reactive Oxygen Species in Atmospheric HULIS by Fe(III) Ions

Chen

Sha

2022

Environ. Sci. Technol.

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Metal ions are key components in atmosphere that potentially affect the optical properties and photochemical reactivity of atmospheric humic-like substances (HULIS), while this mechanism is still unclear. In this study, we demonstrated that atmospheric HULIS coupled with Fe3+, Cu2+, Zn2+, and Al3+ exhibited distinct optical properties and reactive intermediates from that of HULIS utilizing three-dimensional fluorescence spectroscopy and electron paramagnetic resonance spectroscopy. The HULIS components showed light absorption that increased by 56% for the HULIS-Fe3+ system, fluorescence blue shift, and fluorescence quenching, showing a certain dose–effect relationship. These are mainly attributed to the fact that the highly oxidative HULIS chromophores have a stronger complexing ability with Fe3+ ions than the other metal ions. In addition, triplet organics (promoting ratio: 53%) and reactive oxygen species (promoting ratio: 82.6%) in the HULIS-Fe3+ system showed obvious generation promotion. Therefore, the main assumption of the photochemical mechanisms of atmospheric HULIS in the HULIS-Fe3+ system is that Fe3+ ions can form 3HULIS*-Fe3+ complexation with photoexcited 3HULIS* and then transition to the ground state through energy transfer, electron transfer, or nonradiative transition, accompanied by the formation of singlet oxygen and hydroxyl radicals. Our results provide references for evaluating the radiative forcing and aging effect of metal ions on atmospheric aerosols.

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“…Specific absorbance can also be considered as an effective indicator of the origin of HULIS in ambient particulate matter (PM) [2]. HULIS might also threaten human health owing to the production of reactive oxygen species (ROS) or via complexation with transition metals (e.g., Fe, Mn, Cu) [3][4][5]. Recently, many studies have focused on the ROS-generation potential of HULIS in PM 2.5 [6,7].…”

Section: Introductionmentioning

confidence: 99%

Chemical and Optical Characteristics and Sources of PM2.5 Humic-Like Substances at Industrial and Suburban Sites in Changzhou, China

Tao

Sun

et al. 2021

Atmosphere

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The chemical and optical properties and sources of atmospheric PM2.5 humic-like substances (HULIS) were investigated from October to December 2016 in both industrial and suburban areas in Changzhou, China, during polluted and fair days. The average PM2.5 concentration in the industrial region was 113.06 (±64.3) μg m−3, higher than 85.27 (±41.56) μg m−3 at the suburban site. The frequency of polluted days was significantly higher in the industrial region. In contrast, the chemical compositions of PM2.5 at the two sampling sites exhibited no statistically significant differences. Rapidly increased secondary inorganic ions (SNA = NH4+ + SO42− + NO3−) concentrations suggested secondary formation played an important role in haze formation. The daily mean concentration of humic-like substance (HULIS) was 1.8–1.9 times that of HULIS-C (the carbon content of HULIS). Our results showed that HULIS accounted for a considerable fraction of PM2.5 (industrial region: 6.3% vs. suburban region: 9.4%). There were no large differences in the mass ratios of HULIS-C/WSOC at the two sites (46% in the industrial region and 52% in the suburban region). On average, suburban HULIS-C constituted 35.1% of organic carbon (OC), higher than that (21.1%) in the industrial region. Based on different MAE (mass absorption efficiency) values under different pollution levels, we can infer that the optical properties of HULIS varied with PM levels. Moreover, our results showed no distinct difference in E2/E3 (the ratio of light absorbance at 250 nm to that at 365 nm) and AAE300–400 (Absorption Angstrom Exponent at 300–400 nm) for HULIS and WSOC. the MAE365 (MAE at 365 nm) value of HULIS-C was different under three PM2.5 levels (low: PM2.5 < 75 μg m−3, moderate: PM2.5 = 75–150 μg m−3, high: PM2.5 > 150 μg m−3), with the highest MAE365 value on polluted days in the industrial region. Strong correlations between HULIS-C and SNA revealed that HULIS might be contributed from secondary formation at both sites. In addition, good correlations between HULIS-C with K+ in the industrial region implied the importance of biomass burning to PM2.5-bound HULIS. Three common sources of HULIS-C (i.e., vehicle emissions, biomass burning, and secondary aerosols) were identified by positive matrix factorization (PMF) for both sites, but the contributions were different, with the largest contribution from biomass burning in the industrial region and secondary sources in the suburban region, respectively. The findings presented here are important in understanding PM2.5 HULIS chemistry and are valuable for future air pollution control measures.

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A characterization of HULIS-C and the oxidative potential of HULIS and HULIS-Fe(II) mixture in PM2.5 during hazy and non-hazy days in Shanghai

Cited by 28 publications

References 40 publications

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM_2.5

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM_2.5

Significant Promotion of Light Absorption Ability and Formation of Triplet Organics and Reactive Oxygen Species in Atmospheric HULIS by Fe(III) Ions

Chemical and Optical Characteristics and Sources of PM2.5 Humic-Like Substances at Industrial and Suburban Sites in Changzhou, China

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A characterization of HULIS-C and the oxidative potential of HULIS and HULIS-Fe(II) mixture in PM2.5 during hazy and non-hazy days in Shanghai

Cited by 28 publications

References 40 publications

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM2.5

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM2.5

Significant Promotion of Light Absorption Ability and Formation of Triplet Organics and Reactive Oxygen Species in Atmospheric HULIS by Fe(III) Ions

Chemical and Optical Characteristics and Sources of PM2.5 Humic-Like Substances at Industrial and Suburban Sites in Changzhou, China

Contact Info

Product

Resources

About

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM_2.5

On the Relative Contribution of Iron and Organic Compounds, and Their Interaction in Cellular Oxidative Potential of Ambient PM_2.5