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Environmental and health risks of VOCs in the longest inner–city tunnel in Xi’an, Northwest China: Implication of impact from new energy vehicles
2021
Xu, Hongmei | Feng, Rong | Wang, Zexuan | Zhang, Ningning | Zhang, Renjian | He, Kailai | Wang, Qiyuan | Zhang, Qian | Sun, Jian | Zhang, Bin | Shen, Zhenxing | Ho, Steven Hang Sai | Cao, Junji
Traffic source–dominated volatile organic compound (VOC) samples were collected during four time-intervals in a day (Ⅰ: 7:30–10:30, Ⅱ: 11:00–14:00, Ⅲ: 16:30–19:30, and Ⅳ: 20:00–23:00) in a tunnel in summer, 2019, in Xi’an, China. The total measured VOC (TVOC) in periods Ⅰ and Ⅲ (rush hours, 107.2 ± 8.2 parts per billion by volume [ppbv]) was 1.8 times that in periods Ⅱ and Ⅳ (non-rush hours, 58.6 ± 13.8 ppbv), consistent with the variation in vehicle numbers in the tunnel. The considerably elevated ethane and ethylbenzene levels could have been attributed to emissions from compressed natural gas vehicles and the rapid development of methanol-fueled taxis in Xi’an in 2019. The mixing ratios of benzene, toluene, ethylbenzene, and xylenes (BTEX) contributed 9.4%–12.7% to TVOCs, and the contributions were nearly 40% higher in periods Ⅰ and Ⅲ than in Ⅱ and Ⅳ, indicating that BTEX levels were strongly affected by vehicle emissions. The indicators of motor vehicle emission, namely ethylene, propylene, toluene, m/p-xylenes, o-xylene, and propane, contributed to more than half of the ozone formation potential in this study. The noncarcinogenic risks of VOCs in this study were within the international safety standard, whereas the carcinogenic risks exceeded the standard by 2.3–4.6 times, suggesting that carcinogenic risks were more serious than noncarcinogenic risks. VOCs presented 2.2 and 1.4 times noncarcinogenic and carcinogenic risks during rush hours than during non-rush hours, respectively. Notably, the carcinogenic risk in period Ⅳ was comparable with that in period Ⅲ; however, the vehicle numbers and VOC mixing ratios were the lowest at night, which may have attributed to the increasing number and proportion of methanol M100-fueled vehicles in the tunnel. Therefore, VOCs emitted by new energy vehicles should also be seriously considered while evaluating fossil fuel vehicle emissions.
显示更多 [+] 显示较少 [-]Magnetic poly(β-cyclodextrin) combined with solubilizing agents for the rapid bioaccessibility measurement of polycyclic aromatic hydrocarbons in soils
2021
Qin, Shibin | Qi, Shihua | Li, Xiaoshui | Shi, Qiuyun | Li, Huan | Mou, Xiaoxuan | Zhang, Yuan
The rapid determination of the bioaccessibility of polycyclic aromatic hydrocarbons (PAHs) in soils is challenging due to their slow desorption rates and the insufficient extraction efficiency of the available methods. Herein, magnetic poly(β-cyclodextrin) microparticles (Fe₃O₄@PCD) were combined with hydroxypropyl-β-cyclodextrin (HPCD) or methanol (MeOH) as solubilizing agents to develop a rapid and effective method for the bioaccessibility measurement of PAHs. Fe₃O₄@PCD was first validated for the rapid and quantitative adsorption of PAHs from MeOH and HPCD solutions. The solubilizing agents were then coupled with Fe₃O₄@PCD to extract PAHs from soil-water slurries, affording higher extractable fractions than the corresponding solution extraction and comparable to or higher than single Fe₃O₄@PCD or Tenax extraction. The desorption rates of labile PAHs could be markedly accelerated in this process, which were 1.3–12.0 times faster than those of single Fe₃O₄@PCD extraction. Moreover, a low HPCD concentration was sufficient to achieve a strong acceleration of the desorption rate without excessive extraction of the slow desorption fraction. Finally, a comparison with a bioaccumulation assay revealed that the combination of Fe₃O₄@PCD with HPCD could accurately predict the PAH concentration accumulated in earthworms in three field soil samples, indicating that the method is a time-saving and efficient procedure to measure the bioaccessibility of PAHs.
显示更多 [+] 显示较少 [-]Assessing the regional biogenic methanol emission from spring wheat during the growing season: A Canadian case study
2021
Cai, Mengfan | An, Chunjiang | Guy, Christophe | Lü, Chen | Mafakheri, Fereshteh
As a volatile organic compound existing in the atmosphere, methanol plays a key role in atmospheric chemistry due to its comparatively high abundance and long lifetime. Croplands are a significant source of biogenic methanol, but there is a lack of systematic assessment for the production and emission of methanol from crops in various phases. In this study, methanol emissions from spring wheat during the growing period were estimated using a developed emission model. The temporal and spatial variations of methanol emissions of spring wheat in a Canadian province were investigated. The averaged methanol emission of spring wheat is found to be 37.94 ± 7.5 μg·m⁻²·h⁻¹, increasing from north to south and exhibiting phenological peak to valley characteristics. Moreover, cold crop districts are projected to be with higher increase in air temperature and consequent methanol emissions during 2020–2099. Furthermore, the seasonality of methanol emissions is found to be positively correlated to concentrations of CO, filterable particulate matter, and PM₁₀ but negatively related to NO₂ and O₃. The uncertainty and sensitivity analysis results suggest that methanol emissions show a Gamma probabilistic distribution, and growth length, air temperature, solar radiation and leafage are the most important influencing variables. In most cases, methanol emissions increase with air temperature in the range of 3–35 °C while the excessive temperature may result in decreased methanol emissions because of inactivated enzyme activity or increased instant methanol emissions due to heat injury. Notably, induced emission might be the major source of biogenic methanol of mature leaves. The results of this study can be used to develop appropriate strategies for regional emission management of cropping systems.
显示更多 [+] 显示较少 [-]Biomass utilization and production of biofuels from carbon neutral materials
2021
Srivastava, Rajesh K. | Shetti, Nagaraj P. | Reddy, Kakarla Raghava | Kwon, Eilhann E. | Nadagouda, Mallikarjuna N. | Aminabhavi, Tejraj M.
The availability of organic matters in vast quantities from the agricultural/industrial practices has long been a significant environmental challenge. These wastes have created global issues in increasing the levels of BOD or COD in water as well as in soil or air segments. Such wastes can be converted into bioenergy using a specific conversion platform in conjunction with the appropriate utilization of the methods such as anaerobic digestion, secondary waste treatment, or efficient hydrolytic breakdown as these can promote bioenergy production to mitigate the environmental issues. By the proper utilization of waste organics and by adopting innovative approaches, one can develop bioenergy processes to meet the energy needs of the society. Waste organic matters from plant origins or other agro-sources, biopolymers, or complex organic matters (cellulose, hemicelluloses, non-consumable starches or proteins) can be used as cheap raw carbon resources to produce biofuels or biogases to fulfill the ever increasing energy demands. Attempts have been made for bioenergy production by biosynthesizing, methanol, n-butanol, ethanol, algal biodiesel, and biohydrogen using different types of organic matters via biotechnological/chemical routes to meet the world’s energy need by producing least amount of toxic gases (reduction up to 20–70% in concentration) in order to promote sustainable green environmental growth. This review emphasizes on the nature of available wastes, different strategies for its breakdown or hydrolysis, efficient microbial systems. Some representative examples of biomasses source that are used for bioenergy production by providing critical information are discussed. Furthermore, bioenergy production from the plant-based organic matters and environmental issues are also discussed. Advanced biofuels from the organic matters are discussed with efficient microbial and chemical processes for the promotion of biofuel production from the utilization of plant biomasses.
显示更多 [+] 显示较少 [-]A new experimental setup for measuring greenhouse gas and volatile organic compound emissions of silage during the aerobic storage period in a special silage respiration chamber
2020
Krommweh, Manuel S. | Schmithausen, Alexander J. | Deeken, Hauke F. | Büscher, Wolfgang | Maack, Gerd-Christian
The aim of this study was to develop a new experimental setup to determine parallel the emissions of greenhouse gases (GHG) and volatile organic compounds (VOCs) from silage during the opening as well as the subsequent aerobic storage phase of the complete bale without wrapping film. For this purpose, a special silage respiration chamber was used in which a silage bale could be examined. The gas analysis (CO₂, methanol, ethanol, ethyl acetate) of inlet, ambient and outlet air of the silage respiration chamber was carried out by photoacoustic spectroscopy. The gas samples taken inside the bale were analysed by gas chromatography for CO₂, O₂, CH₄, and N₂O. Three silage bales (grass and lucerne) as the smallest silage unit commonly used in practice were examined. The emission behaviour of the bales was recorded during experimental periods up to 55 days. The results allow a differentiation of the outgassing processes. On the one hand, gases produced during the anaerobic ensiling process (CO₂, CH₄, N₂O) are released once in a large amount during the first experimental hours after opening the silage. On the other hand, a continuous outgassing process takes place, which is particularly true for the VOCs ethanol, methanol, and ethyl acetate, whereby VOC emissions increase with rising ambient air temperatures. In this study, the emissions during the first 600 experimental hours from the grass silage bale and lucerne silage bale were 2313 g and 2612 g CO₂, 17.6 g and 145.2 g methanol, 132.3 g and 675.9 g ethanol, 55.1 g and 66.2 g ethyl acetate, respectively. Nevertheless, the focus of this study was on the technical recording of gas concentrations inside the silage bale itself and the emissions in the ambient air of the bale. For a better interpretation of the data, additional factors should be considered in further investigations.
显示更多 [+] 显示较少 [-]Sources of oxygenated volatile organic compounds (OVOCs) in urban atmospheres in North and South China
2020
Huang, Xiao Feng | Zhang, Bin | Xia, Shi-Yong | Han, Yu | Wang, Chuan | Yu, Guang-He | Feng, Ning
Oxygenated volatile organic compounds (OVOCs) are critical precursors of atmospheric ozone (O₃) and secondary organic aerosols (SOA). Although China is experiencing increasing O₃ pollution from north to south, understanding the major sources of OVOCs in this region is still limited due to their active photochemical behaviors. In this study, five critical OVOCs at a northern urban site (Beijing) and a southern urban site (Shenzhen) were monitored in summer using proton transfer reaction-mass spectrometry (PTR-MS). The mean total concentration of VOCs measured in Beijing (39.4 ppb) was much higher than that measured in Shenzhen (16.7 ppb), with methanol and formaldehyde being the most abundant in concentration at both sites. The source apportionment of daytime OVOCs was conducted effectively using a photochemical age-based parameterization method. Biogenic and anthropogenic secondary sources were the main sources of formaldehyde, acetaldehyde, and acetone at both sites, with a total contribution of 46–82%; acetone also had a large regional-scale background contribution (36–38%); methanol and methyl ethyl ketone (MEK) were mainly derived from anthropogenic primary sources (35–55%) at both sites. In addition, the regional background levels of OVOCs measured in North China were shown to be much higher than those measured in South China. The calculation of the total O₃ formation potential (OFP) of OVOCs highlights the comparable contributions from anthropogenic and biogenic sources in both Beijing and Shenzhen, indicating the important role of biogenic OVOC sources even in polluted environments. Since biogenic sources are already important but uncontrollable, anthropogenic emissions in China need to be restricted even more critically in the future.
显示更多 [+] 显示较少 [-]Origin and properties of soluble brown carbon in freshly emitted and aged ambient aerosols over an urban site in India
2019
Sarakāra, Cirantana | Venkataraman, Chandra | Yadav, Suman | Phuleria, Harish C. | Chatterjee, Abhijit
This work investigates the absorption properties of soluble brown carbon (BrC), extracted in methanol and water, from ambient aerosol (PM₁₀) samples, collected over an urban background site in Mumbai, India. The diurnal variability was investigated in samples collected in the morning (7–11 a.m.) and afternoon (12–4 p.m.) periods. Absorption properties of BrC (in the 300–600-nm wavelength range) were measured in filter extracts of water-soluble organic carbon (WSOC) and methanol-soluble organic carbon (MSOC). WSOC and MSOC accounted for on average 52% and 77%, respectively, of the measured OC, potentially indicating unextracted BrC and rendering these values the lower bound. Compared with afternoon samples, the morning samples of MSOC and WSOC had increased BrC concentrations and absorption coefficients (bₐbₛ365; 40%–65%). The correlation between bₐbₛ365 and EC, ns-K⁺, and NO₃⁻ in the morning samples indicated contributions from primary sources, including both biomass and vehicular sources. The decreased bₐbₛ365 in the afternoon samples was partly explained by mixing layer dilution, accompanied by a reduction in the concentrations of primary aerosol constituents. Furthermore, in the afternoon samples, ¹HNMR spectroscopy revealed the presence of more oxidized functional groups and significantly higher OC/EC and WSOC/OC ratios, indicating the greater aging of afternoon aerosol. The MAC₃₆₅ (m²gC⁻¹) for both WSOC and MSOC extracts decreased significantly by 20%–34% in the afternoon samples compared with the morning samples, indicating degradation in the absorption properties of the particles and potentially a change in the constituent BrC chromophores.
显示更多 [+] 显示较少 [-]Are there pharmaceutical compounds in sediments or in water? Determination of the distribution coefficient of benzodiazepine drugs in aquatic environment
2019
Nunes, Chalder Nogueira | dos Anjos, Vanessa Egéa | Quináia, Sueli Pércio
Alprazolam, clonazepam and diazepam are drugs belonging to the benzodiazepine class. These drugs might be important environmental contaminants in aquatic media. A total understanding of behavior and fate of drugs in aquatic environment is not available for these and other drugs. Thus, in this work, a complete optimization of sample treatment and extraction of analytes from sediments and water was described, as well a study of sediment/water distribution comparing it with sample characteristics. Ultrasound for 10 min and 3 steps using 3 mL of extraction solvent were chosen as the stirring form for extraction. A methanol/water (1:1) solution pH 12 was the best extraction solvent. Aiming to eliminate interferences, an addition of 10 μL of NaCl 3.06 mol L⁻¹ was necessary after each step of extraction. Sediment and water samples were characterized, presenting different values on physical-chemical parameters. Six distinct sample sets of water and sediments were spiked with each benzodiazepine and analyzed. Kd values varied from 1.4 to 9.2 L kg⁻¹ for clonazepam, 1.8–11.5 L kg⁻¹ for alprazolam and 2.31–12 L kg⁻¹ for diazepam. A principal component analysis showed high dependence on Kd with sample characteristics mainly related to sediments. In the systems, whose sediments presented high levels of clay, silt and organic matter, the drugs presented a great interaction with the solid part of the system, increasing the Kd value. Koc values varied from 149.25 to 634.13 L kg⁻¹ for clonazepam, 186.57–852.48 L kg⁻¹ for alprazolam, and 194.68–1189.81 L kg⁻¹ for diazepam.
显示更多 [+] 显示较少 [-]Dispersion-box modeling investigation of the influences of gasoline, diesel, M85 and E85 vehicle exhaust emission on photochemistry
2019
Gabay, Maor | Tas, Eran
Alternative transportation fuels (ATFs) can reduce air pollution. However, the influence of conventional fuels—diesel and gasoline, and particularly ATFs on photochemical air pollution is not well-characterized, limiting assessments of ATFs and air quality. This is mainly due to frequent use of lumped chemical mechanisms by related atmospheric modeling. Here we hypothesized that applying a chemical mechanism that is specifically developed according to both emission fractions and photochemical ozone creation potential of volatile organic compounds (VOCs) is key to gaining reliable insights into the impact of transportation fuels on photochemistry. We used a heterogeneous chemical mechanism with 927 reactions and relatively detailed emission inventories to specifically meet the requirements for reliable simulation of the effect of exhaust emissions from vehicles fueled by selected model fuels—diesel, gasoline, and mixtures of 15% gasoline with 85% ethanol (E85) or 85% methanol (M85)—on photochemistry. These dispersion-box model simulations revealed a strong influence of atmospheric background balance between VOCs and nitrogen oxides (NOX = [NO] + [NO2]) on the impact of exhaust emissions on photochemistry, with higher tendency toward ozone (O3) formation or destruction for more VOC-limited or NOX-limited conditions, respectively. Accordingly, higher [NOX]/[VOC] exhaust emission, such as from diesel and M85, resulted in lower O3, not only locally but also downwind of the emission. This offers a new perspective and measure for transportation fuel assessment. Rapid conversion of O3 to hydroxyl and hydroperoxyl radicals downwind of the exhaust emission indicates the importance of simulating the impact of road transportation on photochemistry at high spatial and temporal resolution. Peroxyacetyl nitrate formation was more sensitive to VOC emission under VOC-limited conditions than to NOX emission under NOX-limited conditions. Secondary formaldehyde dominated over primary emitted formaldehyde several minutes after emission. These findings should be verified using a 3D modeling study under varying meteorological conditions.
显示更多 [+] 显示较少 [-]Ambient volatile organic compounds (VOCs) in communities of the Athabasca oil sands region: Sources and screening health risk assessment
2018
Bari, Md Aynul | Kindzierski, Warren B.
An investigation of ambient levels and sources of volatile organic compounds (VOCs) and associated public health risks was carried out at two northern Alberta oil sands communities (Fort McKay and Fort McMurray located < 25 km and >30 km from oil sands development, respectively) for the period January 2010–March 2015. Levels of total detected VOCs were comparatively similar at both communities (Fort McKay: geometric mean = 22.8 μg/m³, interquartile range, IQR = 13.8–41 μg/m³); (Fort McMurray: geometric mean = 23.3 μg/m³, IQR = 12.0–41 μg/m³). In general, methanol (24%–50%), alkanes (26%–32%) and acetaldehyde (23%–30%) were the predominant VOCs followed by acetone (20%–24%) and aromatics (∼9%). Mean and maximum ambient concentrations of selected hazardous VOCs were compared to health risk screening criteria used by United States regulatory agencies. The Positive matrix factorization (PMF) model was used to identify and apportion VOC sources at Fort McKay and Fort McMurray. Five sources were identified at Fort McKay, where four sources (oil sands fugitives, liquid/unburned fuel, ethylbenzene/xylene-rich and petroleum processing) were oil sands related emissions and contributed to 70% of total VOCs. At Fort McMurray six sources were identified, where local sources other than oil sands development were also observed. Contribution of aged air mass/regional transport including biomass burning emissions was ∼30% of total VOCs at both communities. Source-specific carcinogenic and non-carcinogenic risk values were also calculated and were below acceptable and safe levels of risk, except for aged air mass/regional transport (at both communities), and ethylbenzene/xylene-rich (only at Fort McMurray).
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