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Human chemical signature: Investigation on the influence of human presence and selected activities on concentrations of airborne constituents
2020
Mitova, Maya I. | Cluse, Camille | Goujon-Ginglinger, Catherine G. | Kleinhans, Samuel | Rotach, Michel | Tharin, Manuel
There is growing evidence that the very presence of human beings in an enclosed environment can impact air quality by affecting the concentrations of certain airborne volatile organic compounds (VOC). This influence increases considerably when humans perform different activities, such as using toiletries, or simply eating and drinking. To understand the influence of these parameters on the concentrations of selected airborne constituents, a study was performed under simulated residential conditions in an environmentally-controlled exposure room. The human subjects either simply remained for a certain time in the exposure room, or performed pre-defined activities in the room (drinking wine, doing sport, using toiletries, and preparation of a meal containing melted cheese). The impact of each activity was assessed separately using our analytical platform and exposure room under controlled environmental conditions. The results showed that prolonged human presence leads to increased levels of isoprene, TVOCs, formaldehyde and, to a lesser extent, acetaldehyde. These outcomes were further supported by results of meta-analyses of data acquired during several internal studies performed over two years. Furthermore, it was seen that the indoor concentrations of several of the selected constituents rose when the recreational and daily living activities were performed. Indeed, an increase in acetaldehyde was observed for all tested conditions, and these higher indoor levels were especially notable during wine-drinking as well as cheese meal preparation. Formaldehyde increased during the sessions involving sport, using toiletries, and cheese meal preparation. Like acetaldehyde, acrolein, crotonaldehyde and particulate matter levels rose significantly during the cheese meal preparation session. In conclusion, prolonged human residence indoors and some recreational and daily living activities caused substantial emissions of several airborne pollutants under ventilation typical for residential environments.
اظهر المزيد [+] اقل [-]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.
اظهر المزيد [+] اقل [-]Comparative health risk assessment of in-vehicle exposure to formaldehyde and acetaldehyde for taxi drivers and passengers: Effects of zone, fuel, refueling, vehicle's age and model
2019
This study aimed to assess the carcinogenic and non-carcinogenic risks of in-vehicle exposure in Tehran, Iran to formaldehyde and acetaldehyde for different models of taxis, and to explore the effects of city zone, taxi vehicle type, the taxi's age (<1, 1–5, 5–10), fuel type (gasoline, CNG, and LPG), and refueling activities on the estimated health risks based on previously measured concentrations. The overall and age-specific carcinogenic and non-carcinogenic risks of these compounds for taxi drivers and passengers were estimated separately using Monte Carlo simulations. Three scenarios of exposure frequency were defined for taxis commuting in different zones of city: Restricted Traffic Zone (RTZ) and Odd-Even Zone (OEZ) as two plans to reduce air pollution, and no-restriction zone (NRZ). The carcinogenic risks for drivers and passengers, the average risks of formaldehyde and acetaldehyde for most cases were above the 1 × 10⁻⁴. The health risks were greater in Restricted Traffic Zone (RTZ) and Odd-Even Zone (OEZ) in comparison to no-restriction zone (NRZ). The carcinogenic risk from formaldehyde exposures were higher than those for acetaldehyde in all cases. Taxis fueled with LPG showed lower cancer risks for both acetaldehyde and formaldehyde. Refueling increased the carcinogenic risk from both compounds. For non-carcinogenic risks from acetaldehyde, the average hazard ratios for both drivers and passengers were >1, indicating a non-negligible risk. Cancer and non-cancer risks for the taxi drivers were greater than the passengers given the higher time of occupancy. The present study showed that transportation in taxis can impose significant long-term health risks to both passengers and drivers. Development and investment in cleaner choices for public transportations are required.
اظهر المزيد [+] اقل [-]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).
اظهر المزيد [+] اقل [-]Spatiotemporal distribution of carbonyl compounds in China
2015
Ho, K.F. | Ho, Steven Sai Hang | Huang, R.-J. | Dai, W.T. | Cao, J.J. | Tian, Linwei | Deng, W.J.
A sampling campaign was carried out at nine Chinese cities in 2010/2011. Fifteen monocarbonyls (C# = 1–9) were quantified. Temperature is the rate-determining factor of the summertime carbonyl levels. The carbonyl emissions in winter are mainly driven by the primary anthropogenic sources like automobile. A molar ratio of propionaldehyde to nonaldehyde is a barometer of the impact of atmospheric vegetation emission which suggesting that strong vegetation emissions exist in summer and high propionaldehyde abundance is caused by fossil fuel combustion in winter. Potential health risk assessment of formaldehyde and acetaldehyde was conducted and the highest cumulative risks were observed at Chengdu in summer and Wuhan in winter. Because of the strong photochemical reaction and large amount of anthropogenic emissions, high concentrations of carbonyl compounds were observed in Chengdu. The use of ethanol-blended gasoline in Wuhan is the key reason of acetaldehyde emission and action should be taken to avoid potential health risks.
اظهر المزيد [+] اقل [-]Atmospheric fate of peroxyacetyl nitrate in suburban Hong Kong and its impact on local ozone pollution
2019
Zeng, Lewei | Fan, Gang-Jie | Lyu, Xiaopu | Guo, Hai | Wang, Jia-Lin | Yao, Dawen
Peroxyacetyl nitrate (PAN) is an important reservoir of atmospheric nitrogen, modulating reactive nitrogen cycle and ozone (O3) formation. To understand the origins of PAN, a field measurement was conducted at Tung Chung site (TC) in suburban Hong Kong from October to November 2016. The average level of PAN was 0.63 ± 0.05 ppbv, with a maximum of 7.30 ppbv. Higher PAN/O3 ratio (0.043–0.058) was captured on episodes, i.e. when hourly maximum O3 exceeded 80 ppbv, than on non-episodes (0.01), since O3 production was less efficient than PAN when there was an elevation of precursors (i.e. volatile organic compounds (VOCs) and nitrogen oxide (NOx)). Model simulations revealed that oxidations of acetaldehyde (65.3 ± 2.3%), methylglyoxal (MGLY, 12.7 ± 1.2%) and other oxygenated VOCs (OVOCs) (8.0 ± 0.6%), and radical cycling (12.2 ± 0.8%) were the major production pathways of peroxyacetyl (PA) radical, while local PAN formation was controlled by both VOCs and nitrogen dioxide (NO2). Among all VOC species, carbonyls made the highest contribution (59%) to PAN formation, followed by aromatics (26%) and biogenic VOCs (BVOCs) (10%) through direct oxidation/decomposition. Besides, active VOCs (i.e. carbonyls, aromatics, BVOCs and alkenes/alkynes) could stimulate hydroxyl (OH) production, thus indirectly facilitating the PAN formation. Apart from primary emissions, carbonyls were also generated from oxidation of first-generation precursors, i.e., hydrocarbons, of which xylenes contributed the most to PAN production. Furthermore, PAN formation suppressed local O3 formation at a rate of 2.84 ppbv/ppbv, when NO2, OH and hydroperoxy (HO2) levels decreased and nitrogen monoxide (NO) value enhanced. Namely, O3 was reduced by 2.84 ppbv per ppbv PAN formation. Net O3 production rate was weakened (∼36%) due to PAN photochemistry, so as each individual production and loss pathway. The findings advanced our knowledge of atmospheric PAN and its impact on O3 production.
اظهر المزيد [+] اقل [-]Exploration of sources of OVOCs in various atmospheres in southern China
2019
Huang, Xiao Feng | Wang, Chuan | Zhu, Bo | Lin, Li-Liang | He, Ling-Yan
Oxygenated volatile organic compounds (OVOCs) are critical atmospheric ozone and secondary organic aerosol (SOA) precursors and radical sources, while understanding of OVOC sources in the atmosphere, especially with large anthropogenic emissions, still has large uncertainties. A high-sensitivity proton transfer reaction mass spectrometer (PTR-MS) was deployed in vastly different atmospheres in southern China, including an urban site (SZ-U), a regional site (NA-R), and a background site (NL-B). Four critical OVOCs, i.e., methanol, acetone, methyl ethyl ketone (MEK) and acetaldehyde, five groups of aromatic hydrocarbons, isoprene and acetonitrile were measured with a high time resolution. The featured relative abundance and diurnal variations of the OVOCs indicated that methanol, acetone and MEK had prominent contributions from urban industrial activities, while acetaldehyde was closely related to the photochemical formation at all three sites. The photochemical age-based parameterization method was improved locally and then applied to quantify different sources of daytime OVOCs: anthropogenic secondary and biogenic sources (together 60–73%) were always the dominant source for acetaldehyde in various atmospheres; in addition to a significant background for methanol, acetone and MEK, anthropogenic primary emissions (mostly industrial) were their dominant source at SZ-U (38–73%), while biogenic sources played the key role for them at NL-B (30–43%); biomass burning contributed a small fraction of 5–17% for the four OVOCs at the three sites.
اظهر المزيد [+] اقل [-]Multisize particulate matter and volatile organic compounds in arid and semiarid areas of Northwest China
2022
Zhou, Xi | Li, Zhongqin | Zhang, Tingjun | Wang, Feiteng | Tao, Yan | Zhang, Xin
To investigate the chemical components, sources, and interactions of particulate matter (PM) and volatile organic compounds (VOCs), a field campaign was implemented during the spring of 2018 in nine cities in northwestern (NW) China. PM was mainly contributed by organic matter and water-soluble inorganic ions (41% for PM₁₀ and approximately 60% for PM₂.₅ and PM₁). Two typical haze patterns were observed: anthropogenic pollution type (AP-type), wherein contributions of sulfate, nitrate, and ammonium (SNA) increased, and dust pollution type (DP-type), wherein contributions of Ca²⁺ increased and SNA decreased. Source appointment suggested that regional sources contributed close to half to PM₂.₅ pollution (40% for AP-type and 50% for DP-type). Thus, sources from regional transport are also important for haze and dust pollution. The ranking of VOC concentrations was methanol > acetaldehyde > formic acid + ethanol > acetone. Compared with other cities, there are higher oxygenated VOCs (OVOCs) and lower aromatics in NW China. The relationships between VOCs and PM were discussed. The dominating secondary organic aerosols (SOA) formation potential precursors were C₁₀–aromatics, xylene, and styrene under low–nitrogen oxide (NOx) conditions, and benzene, C₁₀–aromatics, and toluene dominated under high–NOx conditions. The quadratic polynomial was the most suitable fitting model for their correlation, and the results suggested that VOC oxidations explained 6.1–10.8% and 9.9–20.7% of SOA formation under high–NOx and low–NOx conditions, respectively.
اظهر المزيد [+] اقل [-]Emission drivers and variability of ambient isoprene, formaldehyde and acetaldehyde in north-west India during monsoon season
2020
Mishra, A.K. | Sinha, V.
Isoprene, formaldehyde and acetaldehyde are important reactive organic compounds which strongly impact atmospheric oxidation processes and formation of tropospheric ozone. Monsoon meteorology and the topography of Himalayan foothills cause surface emissions to get rapidly transported both horizontally and vertically, thereby influencing atmospheric processes in distant regions. Further in monsoon, Indo-Gangetic Plain is a major rice growing region of the world and daytime hourly ozone can frequently exceed phytotoxic dose of 40 ppb O₃. However, the sources and ambient variability of these compounds which are potent ozone precursors are unknown. Here, we investigate the sources and photochemical processes driving their emission/formation during monsoon season from a sub-urban site at the foothills of the Himalayas. The measurements were performed in July, August and September using a high sensitivity mass spectrometer. Average ambient mixing ratios (±1σ variability) of isoprene, formaldehyde, acetaldehyde, and the sum of methyl vinyl ketone and methacrolein (MVK+MACR), were 1.4 ± 0.3 ppb, 5.7 ± 0.9 ppb, 4.5 ± 2.0 ppb, 0.75 ± 0.3 ppb, respectively, and much higher than summertime values in May. For isoprene these values were comparable to mixing ratios observed over tropical forests. Surprisingly, despite occurrence of anthropogenic emissions, biogenic emissions were found to be the major source of isoprene with peak daytime isoprene driven by temperature (r ≥ 0.8) and solar radiation. Photo-oxidation of precursor hydrocarbons were the main sources of acetaldehyde, formaldehyde and MVK+MACR. Ambient mixing ratios of all the compounds correlated poorly with acetonitrile (r ≤ 0.2), a chemical tracer for biomass burning suggesting negligible influence of biomass burning during monsoon season. Our results suggest that during monsoon season when radiation and rain are no longer limiting factors and convective activity causes surface emissions to be transported to upper atmosphere, biogenic emissions can significantly impact the remote upper atmosphere, climate and ozone affecting rice yields.
اظهر المزيد [+] اقل [-]Seasonal and diurnal characteristics of carbonyls in the urban atmosphere of Changsha, a mountainous city in south-central China
2019
Jiang, Zhaohui | Zheng, Xuan | Zhai, Haiqing | Wang, Yujiao | Wang, Qiong | Yang, Zhishu
Seasonal and diurnal variations of carbonyl compounds were investigated in the ambient air of a mountainous city in China, from September 2014 to July 2015. The most abundant carbonyl compounds are formaldehyde, acetaldehyde and acetone, propionaldehyde and methacryladehyde (MACR), which were all measured in most samples. The average concentrations of formaldehyde, acetaldehyde, acetone, propionaldehyde and MACR in the atmosphere in Changsha were broken down into each season: 6.57, 3.29, 3.66, 0.67 and 0.54 μg/m³ respectively during Spring, 14.09, 8.28, 9.02, 1.28 and 0.6 μg/m³, respectively during Summer, 9.24, 5.48, 8.62, 0.73 and 0.62 μg/m³, respectively during Autumn, and 5.88, 4.84, 7.84, 0.87 and 0.26 μg/m³ respectively during Winter. And majority of the species had higher concentration during noon, showing photochemical oxidation and human activities played an important role in diurnal variation. The highest average C1/C2 (formaldehyde/acetaldehyde) ratio was observed in summer (2.10) compared to those (1.33–2.03) in other seasons, implying the photochemical activities had a positive effect on increasing the ratio of C1/C2. In this study, the monthly concentration of formaldehyde produced from isoprene accounts for 4.8%–39.1% of formaldehyde in ambient air. Strong correlation among some carbonyl compounds means that they came from the same sources. Photochemical reaction was the main source of carbonyl compounds in summer and vehicular exhaust (gasoline and diesel engines) in winter. Changsha is not a completely urbanized city and it is rich in vegetation of broadleaf evergreen shrubs. Both atmospheric photochemical reactions and anthropogenic sources, including vehicular exhaust and industrial processes, dominate the levels of carbonyls. The ILTCR and HQ values of formaldehyde and acetaldehyde are 1.23E-04 and 1.34E-05, 2.80E-01 and 1.86E-01, respectively.
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