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Formation mechanism of secondary organic aerosol from ozonolysis of gasoline vehicle exhaust
2018
Yang, Bo | Ma, Pengkun | Shu, Jinian | Zhang, Peng | Huang, Jingyun | Zhang, Haixu
Gasoline vehicles are a major source of anthropogenic secondary organic aerosols (SOAs). However, current models based on known precursors fail to explain the substantial SOAs from vehicle emissions due to the inadequate understanding of the formation mechanism. To provide more information on this issue, the formation of SOAs from ozonolysis of four light-duty gasoline vehicle exhaust systems was investigated with a vacuum ultraviolet photoionization mass spectrometer (VUV-PIMS). Remarkable SOAs formation was observed and the SOAs were primarily aliphatic alkenes. PI mass spectra of the SOAs from all vehicles exhibited similar spectral patterns (a regular mass group with m/z at 98, 112, 126 …). Interestingly, most carbonyl products of aliphatic alkenes observed as major gaseous products have specific molecular weights, and the main formation pathway of SOAs can be explained well using aldol condensation reactions of these carbonyls. This is a direct observation of the aldol condensation as a dominated pathway for SOAs formation, and the first report on the composition and formation mechanism of the SOAs from the ozonolysis of gasoline vehicle exhaust is given. The study reveals that low molecular weight alkenes may play a more significant role in vehicle-induced SOAs formation than previously believed. More importantly, the PI mass spectra of SOAs from vehicles show similarities to the field aerosol sample mass spectra, suggesting the possible significance of the aldol condensation reactions in ambient aerosol formation. Since carbonyls are a major degradation product of biogenic and anthropogenic VOCs through atmospheric oxidation processes, the mechanism proposed in this study can be applied more generally to explain aerosol formation from the oxidation of atmospheric hydrocarbons.
Show more [+] Less [-]One-century sedimentary record of heavy metal pollution in western Taihu Lake, China
2018
Li, Yan | Zhou, Shenglu | Zhu, Qing | Li, Baojie | Wang, Junxiao | Wang, Chunhui | Chen, Lian | Wu, Shaohua
Long-term trends of sediment compositions are important for assessing the impact of human activities on the sediment and protecting the sediment environment. In this study, based on the contents of heavy metals and the Pb isotope ratios in lake sediments, atmospheric dustfall and soil in Yixing, China, the representative heavy metals (Zn, Pb, Cr and Cd) in lake sediments from western Taihu Lake were studied. The evolution history of heavy metals in the local environment was constructed for the past 100 years. From 1892 to the 1990s, the anthropogenic fluxes of the representative heavy metals were negligible, indicating minimal anthropogenic emissions of heavy metals. Since the 1990s, anthropogenic fluxes of the representative heavy metals began to increase, concurrent with the economic growth and development in the western Taihu Lake Basin after the Chinese economic reform. The maximum flux percentage of the heavy metals in the sediments, caused by human activities, is 23.0% for Zn, 31.6% for Pb, 39.5% for Cr and 85.3% for Cd, indicating that most of the Cd comes from human activities. The Cd content in the western Taihu Lake Basin was significantly higher than that in the other areas, and the rapid development of the industry in the western Taihu Lake Basin and ceramics in Yixing led to the enrichment of heavy metals in local sediments. Since the 21st century, measures have been taken to control the pollution of heavy metals, including the increase in local government attention and the deployment of environmental monitoring technology. However, heavy metal content remains high, and the Pb content is still increasing. The ratios of Pb isotopes show that the main sources of heavy metals in the western Taihu Lake sediments, the local soil of Yixing and the atmospheric dustfall are coal combustion, leaded gasoline combustion, industrial wastewater and domestic sewage.
Show more [+] Less [-]Volatile organic compounds in stormwater from a community of Beijing, China
2018
Li, Haiyan | Wang, Youshu | Liu, Fei | Tong, Linlin | Li, Kun | Yang, Hua | Zhang, Liang
Stormwater samples were collected from six different land use sites with three time-intervals during a precipitation event on August 12, 2016, from a community of Beijing, China. A total of 46 species volatile organic compounds (VOCs) were detected in these stormwater samples, including methyl tertiary-butyl ether (MTBE), aromatic hydrocarbons, halogenated aromatics, Halogenated alkanes, and alkenes. The total VOC concentrations varied in the six sites following order: highway junction > city road > gas station > park > campus > residential area, except for MTBE, which was much higher at gas station compared to other land use sites. ANOVA results indicated both land use and precipitation time intervals could significantly affect the VOC concentrations even in the small area. The Beijing atmospheric VOC concentrations were too low to explain the high concentrations in stormwater, suggesting that land surfaces may be the main sources of VOC other than the ambient atmosphere. MTBE and other VOCs correlation analysis indicated that MTBE mostly came from gasoline emissions, spills or vehicle exhausts, whereas the BTEX (benzene, toluene, ethylbenzene, Xylenes) and the halogenated aromatics were transferred from chemical plants through land surfaces accumulating and the wind blowing atmospheric VOCs. Xylenes/ethylbenzene (X/E) ratios variations indicated that stormwater incorporated larger amount of fresh emitted air during the precipitation event than prior to it. Information of these stormwater VOCs in this study could be used in the community pollution reduction strategies.
Show more [+] Less [-]Assessment of lung cell toxicity of various gasoline engine exhausts using a versatile in vitro exposure system
2018
Bisig, Christoph | Comte, Pierre | Güdel, Martin | Czerwiński, Janusz | Mayer, Andreas | Müller, Loretta | Petri-Fink, Alke | Rothen-Rutishauser, Barbara
Adverse effect studies of gasoline exhaust are scarce, even though gasoline direct injection (GDI) vehicles can emit a high number of particles.The aim of this study was to conduct an in vitro hazard assessment of different GDI exhausts using two different cell culture models mimicking the human airway. In addition to gasoline particle filters (GPF), the effects of two lubrication oils with low and high ash content were assessed, since it is known that oils are important contributors to exhaust emissions.Complete exhausts from two gasoline driven cars (GDI1 and GDI2) were applied for 6 h (acute exposure) to a multi-cellular human lung model (16HBE14o-cell line, macrophages, and dendritic cells) and a primary human airway model (MucilAir™). GDI1 vehicle was driven unfiltered and filtered with an uncoated and a coated GPF. GDI2 vehicle was driven under four settings with different fuels: normal unleaded gasoline, 2% high and low ash oil in gasoline, and 2% high ash oil in gasoline with a GPF. GDI1 unfiltered was also used for a repeated exposure (3 times 6 h) to assess possible adverse effects.After 6 h exposure, no genes or proteins for oxidative stress or pro-inflammation were upregulated compared to the filtered air control in both cell systems, neither in GDI1 with GPFs nor in GDI2 with the different fuels. However, the repeated exposure led to a significant increase in HMOX1 and TNFa gene expression in the multi-cellular model, showing the responsiveness of the system towards gasoline engine exhaust upon prolonged exposure.The reduction of particles by GPFs is significant and no adverse effects were observed in vitro during a short-term exposure. On the other hand, more data comparing different lubrication oils and their possible adverse effects are needed. Future experiments also should, as shown here, focus on repeated exposures.
Show more [+] Less [-]Chemometrics analysis of petroleum hydrocarbons sources in the street dust, runoff and sediment of urban rivers in Anzali port - South of Caspian Sea
2018
Azimi, Ali | Bakhtiari, Alireza Riahi | Tauler, Roma
Major sources of petroleum hydrocarbons in the south of Caspian Sea (Anzali city) have been investigated through an approach which combines Gas Chromatography–Mass Spectrometry with Principal Component Analysis (PCA) and Multivariate Curve Resolution-Alternating Least Squares chemometric methods. Terpane, catagenetic hopane and sterane hydrocarbons were analyzed in the street dust, filtered sediments of runoff, soluble runoff water and river sediment samples as well as in automobiles exhaust, tires, asphalt, engine oil, gasoline and diesel samples, as possible sources of these hydrocarbons. PCA and MCR-ALS results showed that a large part of the analyzed hydrocarbons in street dust, runoffs and in some of the river sediment samples can be explained by the proposed known sources, while the observed variation of hydrocarbon concentrations in many of the river sediment samples was not much affected by the proposed known sources, and they were most probably receiving other pollution sources not included in our study. This study also has shown that results obtained from hydrocarbon marker molecular ratios, to identify petroleum pollution sources in the environments, are in agreement with those obtained from pollution sources resolved by MCR-ALS simultaneous analysis of all samples and variables.
Show more [+] Less [-]Characterizing benzene series (BTEX) pollutants build-up process on urban roads: Implication for the importance of temperature
2018
Liu, An | Hong, Nian | Zhu, Panfeng | Guan, Yuntao
Benzene series (BTEX) pollutants which are generated by traffic can deposit (build-up) on urban road surfaces. When they are washed-off by stormwater runoff, BTEX are toxic to ecological and human health if the stormwater is reused. To understand the risk posed by BTEX, it is essential to have an in-depth investigation on BTEX build-up, one of the most important stormwater pollutant processes. This study analysed the relationship between BTEX build-up and BTEX build-up's influential factors. The outcomes confirmed an important role of climatic factors (particularly temperature) on influencing BTEX build-up. This has not been considered in previous stormwater studies although this has been widely focused in atmospheric pollution. BTEX build-up loads were generally higher and the variability was low in dry seasons with low temperature such as winter and spring. Additionally, the influence of temperature on BTEX build-up on urban road surfaces is more important in the case of larger particles (such as >75 μm) than smaller particles. The study also showed that petrol station areas have a potential to export stormwater runoff with high BTEX concentrations, compared to typical urban roads. This is particularly applicable in winter and spring. These outcomes can provide useful guidance to improving stormwater quality modelling approaches, especially relevant to estimation of BTEX concentrations in the stormwater.
Show more [+] Less [-]Respiratory hazard assessment of combined exposure to complete gasoline exhaust and respirable volcanic ash in a multicellular human lung model at the air-liquid interface
2018
Tomašek, Ines | Horwell, Claire J. | Bisig, Christoph | Damby, David E. | Comte, Pierre | Czerwiński, Janusz | Petri-Fink, Alke | Clift, Martin J.D. | Drasler, Barbara | Rothen-Rutishauser, Barbara
Communities resident in urban areas located near active volcanoes can experience volcanic ash exposures during, and following, an eruption, in addition to sustained exposures to high concentrations of anthropogenic air pollutants (e.g., vehicle exhaust emissions). Inhalation of anthropogenic pollution is known to cause the onset of, or exacerbate, respiratory and cardiovascular diseases. It is further postulated similar exposure to volcanic ash can also affect such disease states. Understanding of the impact of combined exposure of volcanic ash and anthropogenic pollution to human health, however, remains limited.The aim of this study was to assess the biological impact of combined exposure to respirable volcanic ash (from Soufrière Hills volcano (SHV), Montserrat and Chaitén volcano (ChV), Chile; representing different magmatic compositions and eruption styles) and freshly-generated complete exhaust from a gasoline vehicle. A multicellular human lung model (an epithelial cell-layer composed of A549 alveolar type II-like cells complemented with human blood monocyte-derived macrophages and dendritic cells cultured at the air-liquid interface) was exposed to diluted exhaust (1:10) continuously for 6 h, followed by immediate exposure to the ash as a dry powder (0.54 ± 0.19 μg/cm2 and 0.39 ± 0.09 μg/cm2 for SHV and ChV ash, respectively). After an 18 h incubation, cells were exposed again for 6 h to diluted exhaust, and a final 18 h incubation (at 37 °C and 5% CO2). Cell cultures were then assessed for cytotoxic, oxidative stress and (pro-)inflammatory responses.Results indicate that, at all tested (sub-lethal) concentrations, co-exposures with both ash samples induced no significant expression of genes associated with oxidative stress (HMOX1, NQO1) or production of (pro-)inflammatory markers (IL-1β, IL-8, TNF-α) at the gene and protein levels. In summary, considering the employed experimental conditions, combined exposure of volcanic ash and gasoline vehicle exhaust has a limited short-term biological impact to an advanced lung cell in vitro model.
Show more [+] Less [-]Investigation of in-cabin volatile organic compounds (VOCs) in taxis; influence of vehicle's age, model, fuel, and refueling
2018
Bakhtiari, Reza | Hadei, Mostafa | Hopke, Philip K. | Shahsavani, Abbas | Rastkari, Noushin | Kermani, Majid | Yarahmadi, Maryam | Ghaderpoori, Afshin
The air pollutant species and concentrations in taxis' cabins can present significant health impacts on health. This study measured the concentrations of benzene, toluene, ethylbenzene, xylene (BTEX), formaldehyde, and acetaldehyde in the cabins of four different taxi models. The effects of taxi's age, fuel type, and refueling were investigated. Four taxi models in 3 age groups were fueled with 3 different fuels (gas, compressed natural gas (CNG), and liquefied petroleum gas (LPG)), and the concentrations of 6 air pollutants were measured in the taxi cabins before and after refueling. BTEX, formaldehyde, and acetaldehyde sampling were actively sampled using NIOSH methods 1501, 2541, and 2538, respectively. The average BTEX concentrations for all taxi models were below guideline values. The average concentrations (±SD) of formaldehyde in Model 1 to Model 4 taxis were 889 (±356), 806 (±323), 1144 (±240), and 934 (±167) ppbv, respectively. Acetaldehyde average concentrations (±SD) in Model 1 to Model 4 taxis were 410 (±223), 441 (±241), 443 (±210), and 482 (±91) ppbv, respectively. Refueling increased the in-vehicle concentrations of pollutants primarily the CNG and LPG fuels. BTEX concentrations in all taxi models were significantly higher for gasoline. Taxi age inversely affected formaldehyde and acetaldehyde. In conclusion, it seems that refueling process and substitution of gasoline with CNG and LPG can be considered as solutions to improve in-vehicle air concentrations for taxis.
Show more [+] Less [-]Implications of co-contamination with aged heavy metals and total petroleum hydrocarbons on natural attenuation and ecotoxicity in Australian soils
2018
Khudur, Leadin S. | Gleeson, Deirdre B. | Ryan, Megan H. | Shahsavari, Esmaeil | Haleyur, Nagalakshmi | Nugegoda, Dayanthi | Ball, A. S.
The bioremediation of historic industrial contaminated sites is a complex process. Co-contamination, often with lead which was commonly added to gasoline until 16 years ago is one of the biggest challenges affecting the clean-up of these sites. In this study, the effect of heavy metals, as co-contaminant, together with total petroleum hydrocarbons (TPH) is reported, in terms of remaining soil toxicity and the structure of the microbial communities. Contaminated soil samples from a relatively hot and dry climate in Western Australia were collected (n = 27). Analysis of soils showed the presence of both contaminants, TPHs and heavy metals. The Microtox test confirmed that their co-presence elevated the remaining ecotoxicity. Toxicity was correlated with the presence of lead, zinc and TPH (0.893, 0.599 and 0.488), respectively, assessed using Pearson Correlation coefficient factor. Next Generation Sequencing of soil bacterial 16S rRNA, revealed a lack of dominate genera; however, despite the variation in soil type, a few genera including Azospirillum spp. and Conexibacter were present in most soil samples (85% and 82% of all soils, respectively). Likewise, many genera of hydrocarbon-degrading bacteria were identified in all soil samples. Streptomyces spp. was presented in 93% of the samples with abundance between 7% and 40%. In contrast, Acinetobacter spp. was found in only one sample but was a dominant member of (45%) of the microbial community. In addition, some bacterial genera were correlated to the presence of the heavy metals, such as Geodermatophilus spp., Rhodovibrio spp. and Rubrobacter spp. which were correlated with copper, lead and zinc, respectively. This study concludes that TPH and heavy metal co-contamination significantly elevated the associated toxicity. This is an important consideration when carrying out risk assessment associated with natural attenuation. This study also improves knowledge about the dynamics of microbial communities in mixed contamination scenarios.
Show more [+] Less [-]Using an innovative flag element ratio approach to tracking potential sources of heavy metals on urban road surfaces
2018
Hong, Nian | Zhu, Panfeng | Liu, An | Zhao, Xu | Guan, Yuntao
Heavy metals deposited on urban road surfaces can be washed-off by stormwater runoff, undermining stormwater reuse safety due to their high toxicity to ecological and human health. Heavy metals on urban road surfaces come from diverse sources and tracking these sources is essential to effectively manage stormwater and hence its reuse safety. This research study developed an innovative approach to tracking sources of heavy metals using data collected in Shenzhen, China. This approach developed was based on a “flag element ratio” theory, where each source generally corresponds to a specific ratio of targeted pollutants to the flag element. It is noted that Cr, Cu, Pb, Ni, and Zn on urban roads were 19.05 mg/kg to 152.01 mg/kg, 25.66 mg/kg to 310.75 mg/kg, 15.61 mg/kg to 220.35 mg/kg, 10.65 mg/kg to 100.28 mg/kg, and 138.14 mg/kg to 1047.05 mg/kg, respectively. Gasoline emission was the main source for Cr, Ni and Pb, while braking wear and tyre wear were the major sources of Cu and Zn, respectively. Furthermore, the rankings of sources of each heavy metal in terms of their contributions were obtained by using this approach. Vehicle exhaust was found as the main contributor for all the heavy metals on urban road surfaces. This highlighted that vehicle exhaust should be seriously considered in terms of controlling heavy metal pollution on urban road surfaces and hence resulting urban road stormwater runoff.
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