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Polar organic aerosol tracers in two areas in Beijing-Tianjin-Hebei region: Concentration comparison before and in the sept. Third Parade and sources
2021
Li, Li | Wu, Di | Chang, Xing | Tang, Yi | Hua, Yang | Xu, Qingcheng | Deng, Shihuai | Wang, Shuxiao | Hao, Jiming
A total of 106 24-h PM₂.₅ aerosol samples were collected in an urban area (Shijiazhuang, SJZ) and a suburban area (Liulihe, LLH, Fangshan County, Beijing) in the Beijing-Tianjin-Hebei (BTH) region in 2 periods: the first is from 10 July to 10 August, which is before Sept. Third Parade (Period I); the second is from 20 Aug. to 6 Sept. 2015, which is during Sept. Third Parade (Period II). Polar organic tracers, including isoprene, α-pinene, β-caryophyllene and toluene oxidation products, as well as sugars and carboxylic acids were measured. In Period II, rigorous emission-reduction measures were taken in the BTH region. With the anthropogenic emission being cut down significantly, the average concentrations of isoprene, α-pinene, β-caryophyllene and toluene oxidation products and all carboxylic acids (except tetradecanoic, palmitic, and stearic acids), were lower in Period II than those in Period I in LLH, indicating that the SOA tracers were decreased with precursor emission volumes and yields in the atmosphere. Moreover, sugar compounds were shown with comparable levels during the two periods in LLH, suggesting that no measures were taken to reduce the intensities of the biogenic sources. On the contrary, tetradecanoic, palmitic, and stearic acids were shown with obviously higher concentrations in Period II than those in Period I, demonstrating that cooking fumes increased during Sept. Third Parade period.The positive matrix factorization (PMF) model combining with tracer-based method was applied to explore the sources of secondary organic carbon (SOC). It reveals that the sources of SOC include isoprene, α-pinene, β-caryophyllene and toluene oxidation products, fossil fuel combustion, cooking fumes and regionally transferred aged aerosols. These sources accounted for 11.3%, 9.0%, 15.5%, 10.9%, 29.2%, 2.9%, 21.1% of SOC for SJZ, and 12.7%, 11.2%, 9.7%, 14.4%, 25.3%, 0%, 26.7% of SOC for LLH, during the whole sampling periods respectively.
Mostrar más [+] Menos [-]Occurance, emission and environmental effects of non-methane hydrocarbons in the Yellow Sea and the East China Sea
2021
Wu, Ying-Cui | Li, Jian-Long | Wang, Jian | Zhuang, Guang-Chao | Liu, Xi-Ting | Zhang, Hong-Hai | Yang, Gui-Peng
The spatial distributions, fluxes, and environmental effects of non-methane hydrocarbons (NMHCs) were investigated in the Yellow Sea (YS) and the East China Sea (ECS) in spring. The average concentrations of ethane, propane, i-/n-butane, ethylene, propylene and isoprene in the seawater were 18.1 ± 6.4, 15.4 ± 4.7, 6.8 ± 2.9, 6.4 ± 3.2, 67.1 ± 26.7, 20.5 ± 8.7 and 17.1 ± 11.1 pmol L⁻¹, respectively. The alkenes in the surface seawater were more abundant than their saturated homologs and NMHCs concentrations (with the exception of isoprene) decreased with carbon number. The spatial variations of isoprene were consistent with the distributions of chlorophyll a (Chl-a) and Chaetoceros, Skeletonema, Nitzschia mainly contributed to the production of isoprene, while the others’ distributions might be related to their photochemical production. Observations in atmospheric NMHCs indicated alkanes in the marine atmosphere decreased from inshore to offshore due to influence of the continental emissions, while alkenes were largely derived from the oceanic source. In addition, no apparent diurnal discrepancy of atmospheric NMHCs (except for isoprene) were found between daytime and night. As the main sink of NMHCs in seawater, the average sea-to-air fluxes of ethane, propane, i-/n-butane, ethylene and propylene were 31.70, 29.75, 18.49, 15.89, 239.6, 67.94 and 52.41 nmol m⁻² d⁻¹, respectively. The average annual emissions of isoprene accounted for 0.1–1.3% of the global ocean emissions, which indicated that the coastal and shelf areas might be significant sources of isoprene. Furthermore, this study represents the first effort to estimate the environmental effects caused by NMHCs over the YS and the ECS and the results demonstrated contributions of alkanes to ozone and secondary organic aerosol (SOA) formation were lower than those of the alkenes and the largest contributor was isoprene.
Mostrar más [+] Menos [-]Ozone impairs the response of isoprene emission to foliar nitrogen and phosphorus in poplar
2020
Hoshika, Yasutomo | Brilli, Federico | Baraldi, Rita | Fares, Silvano | Carrari, Elisa | Zhang, Lu | Badea, Ovidiu | Paoletti, Elena
Tropospheric ozone (O₃) impairs physiological processes of plants while nitrogen (N) deposition may cause imbalances in soil N and other nutrients such as phosphorus (P) suggesting an increase of P demand for plants. However, the combined effect of O₃, soil N and P on isoprene emission from leaves has never been tested. We therefore examined isoprene emission in leaves of Oxford poplar clone exposed to O₃ (ambient, AA [35.0 nmol mol⁻¹ as daily mean]; 1.5 × AA; 2.0 × AA), soil N (0 and 80 kg N ha⁻¹) and soil P (0, 40 and 80 kg P ha⁻¹) in July and September in a Free-Air Controlled Exposure (FACE) facility. We also investigated the response of isoprene emission to foliar N, P and abscisic acid (ABA) contents in September because the 2-C-methylerythritol-5-phosphate (MEP) pathway of isoprenoid biosynthesis produces ABA. We found that O₃ increased isoprene emission in July, which was associated to increased dark respiration, suggesting an activation of metabolism against O₃ stress as an initial response. However, O₃ decreased isoprene emission in September which was associated to reduced net photosynthesis. In September, isoprene emission was positively correlated with leaf N content and negatively correlated with leaf P content in AA. However, no response of isoprene emission to foliar N and P was found in elevated O₃, suggesting that the isoprene responses to foliar N and P depended on the O₃ exposure levels. Isoprene emission rate in 1.5 × AA and 2.0 × AA increased with increasing leaf ABA content, indicating accelerated senescence of injured leaves to favor new leaf growth when high O₃ and nutritional availability in the soil were combined. Even though foliar N and P usually act as a proxy for isoprene emission rate, the impact of recent abiotic factors such as O₃ should be always considered for modeling isoprene emission under climate change.
Mostrar más [+] Menos [-]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.
Mostrar más [+] Menos [-]Investigation of emission characteristics of NMVOCs over urban site of western India
2019
Yadav, Ravi | Sahu, L.K. | Tripathi, Nidhi | Pal, D. | Beig, G. | Jaaffrey, S.N.A.
This is the first study to characterize the variation and emission of C₂-C₅ non-methane volatile organic compounds (NMVOCs) in a semi-urban site of western India based on measurements during February–December 2015. Anthropogenic NMVOCs show clear seasonal dependence with highest in winter and lowest in monsoon season. Biogenic NMVOCs likes isoprene show highest mixing ratios in the pre-monsoon season. The diurnal variation of NMVOC species can be described by elevated values from night till morning and lower values in the afternoon hours. The elevated levels of NMVOCs during night and early morning hours were caused mainly by weaker winds, temperature inversion and reduced chemical loss. The correlations between NMVOCs, CO and NOx indicate the dominant role of various local emission sources. Use and leakage of liquefied petroleum gas (LPG) contributed to the elevated levels of propane and butanes. Mixing ratios of ethylene, propylene, CO, NOx, etc. show predominant emissions from combustion of fuels in automobiles and industries. The Positive Matrix Factorization (PMF) source apportionments were performed for the seven major emission sectors (i.e. Vehicular exhaust, Mixed industrial emissions, Biomass/Fired brick kilns/Bio-fuel, Petrochem, LPG, Gas evaporation, Biogenic). Emissions from vehicle exhaust and industry-related sources contributed to about 19% and 40% of the NMVOCs, respectively. And the rest (41%) was attributed to the emissions from biogenic sources, LPG, gasoline evaporation and biomass burning. Diurnal and seasonal variations of NMVOCs were controlled by local emissions, meteorology, OH concentrations, long-range transport and planetary boundary layer height. This study provides a good reference for framing environmental policies to improve the air quality in western region of India.
Mostrar más [+] Menos [-]VOC emissions and carbon balance of two bioenergy plantations in response to nitrogen fertilization: A comparison of Miscanthus and Salix
2018
Hu, Bin | Jarosch, Ann-Mareike | Gauder, Martin | Graeff-Hönninger, Simone | Schnitzler, Jörg-Peter | Grote, Rüdiger | Rennenberg, H. (Heinz) | Kreuzwieser, Jürgen
Energy crops are an important renewable source for energy production in future. To ensure high yields of crops, N fertilization is a common practice. However, knowledge on environmental impacts of bioenergy plantations, particularly in systems involving trees, and the effects of N fertilization is scarce. We studied the emission of volatile organic compounds (VOC), which negatively affect the environment by contributing to tropospheric ozone and aerosols formation, from Miscanthus and willow plantations. Particularly, we aimed at quantifying the effect of N fertilization on VOC emission. For this purpose, we determined plant traits, photosynthetic gas exchange and VOC emission rates of the two systems as affected by N fertilization (0 and 80 kg ha−1 yr−1). Additionally, we used a modelling approach to simulate (i) the annual VOC emission rates as well as (ii) the OH. reactivity resulting from individual VOC emitted. Total VOC emissions from Salix was 1.5- and 2.5-fold higher compared to Miscanthus in non-fertilized and fertilized plantations, respectively. Isoprene was the dominating VOC in Salix (80–130 μg g−1 DW h−1), whereas it was negligible in Miscanthus. We identified twenty-eight VOC compounds, which were released by Miscanthus with the green leaf volatile hexanal as well as dimethyl benzene, dihydrofuranone, phenol, and decanal as the dominant volatiles. The pattern of VOC released from this species clearly differed to the pattern emitted by Salix. OH. reactivity from VOC released by Salix was ca. 8-times higher than that of Miscanthus. N fertilization enhanced stand level VOC emissions, mainly by promoting the leaf area index and only marginally by enhancing the basal emission capacity of leaves. Considering the higher productivity of fertilized Miscanthus compared to Salix together with the considerably lower OH. reactivity per weight unit of biomass produced, qualified the C4-perennial grass Miscanthus as a superior source of future bioenergy production.
Mostrar más [+] Menos [-]On the use of an explicit chemical mechanism to dissect peroxy acetyl nitrate formation
2014
Xue, Likun | Wang, Tao | Wang, Xinfeng | Blake, Donald R. | Gao, Jian | Nie, Wei | Gao, Rui | Gao, Xiaomei | Xu, Zheng | Ding, Aijun | Huang, Yu | Lee, Shuncheng | Chen, Yizhen | Wang, Shulan | Chai, Fahe | Zhang, Qingzhu | Wang, Wenxing
Peroxy acetyl nitrate (PAN) is a key component of photochemical smog and plays an important role in atmospheric chemistry. Though it has been known that PAN is produced via reactions of nitrogen oxides (NOx) with some volatile organic compounds (VOCs), it is difficult to quantify the contributions of individual precursor species. Here we use an explicit photochemical model – Master Chemical Mechanism (MCM) model – to dissect PAN formation and identify principal precursors, by analyzing measurements made in Beijing in summer 2008. PAN production was sensitive to both NOx and VOCs. Isoprene was the predominant VOC precursor at suburb with biogenic impact, whilst anthropogenic hydrocarbons dominated at downtown. PAN production was attributable to a relatively small class of compounds including NOx, xylenes, trimethylbenzenes, trans/cis-2-butenes, toluene, and propene. MCM can advance understanding of PAN photochemistry to a species level, and provide more relevant recommendations for mitigating photochemical pollution in large cities.
Mostrar más [+] Menos [-]Effects of elevated ozone on the emission of volatile isoprenoids from flowers and leaves of rose (Rosa sp.) varieties
2021
Yuan, Xiangyang | Feng, Zhaozhong | Hu, Chunfang | Zhang, Kun | Qu, Laiye | Paoletti, Elena
Tropospheric ozone (O₃) affects isoprenoid emissions, and floral emissions in particular, which may result in potential impacts on the interactions of plants with other organisms. The effects of ozone (O₃) on isoprenoid emissions have been investigated for many years, while knowledge on O₃ effects on floral emissions is still scarce and the relevant mechanism has not been clarified so far. We investigated the effects of O₃ on floral and foliar isoprenoid emissions (mainly isoprene, monoterpenes and sesquiterpenes) and their synthase substrates from three rose varieties (CH, Rosa chinensis Jacq. var. chinensis; SA, R. hybrida ‘Saiun’; MO, R. hybrida ‘Monica Bellucci’) at different exposure durations. Results indicated that the O₃-induced stimulation after short-term exposure (35 days after the beginning of O₃ exposure) was significant only for sesquiterpene emissions from flowers, while long-term O₃ exposure (90 days after the beginning of O₃ exposure) significantly decreased both foliar and floral monoterpene and sesquiterpene emissions. In addition, the observed decline of emissions under long-term O₃ exposure resulted from the limitation of synthase substrates, and the responses of emissions and substrates varied among varieties, with the greatest variation in the O₃-sensitive variety. These findings provide important insights on plant isoprenoid emissions and species selection for landscaping, especially in areas with high O₃ concentration.
Mostrar más [+] Menos [-]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.
Mostrar más [+] Menos [-]Source apportionment of fine particulate matter organic carbon in Shenzhen, China by chemical mass balance and radiocarbon methods
2018
Al-Naiema, Ibrahim M. | Yoon, Subin | Wang, Yu-Qin | Zhang, Yuan-Xun | Sheesley, Rebecca J. | Stone, Elizabeth A.
Chemical mass balance (CMB) modeling and radiocarbon measurements were combined to evaluate the sources of carbonaceous fine particulate matter (PM2.5) in Shenzhen, China during and after the 2011 summer Universiade games when air pollution control measurements were implemented to achieve air quality targets. Ambient PM2.5 filter samples were collected daily at two sampling sites (Peking University Shenzhen campus and Longgang) over 24 consecutive days, covering the controlled and uncontrolled periods. During the controlled period, the average PM2.5 concentration was less than half of what it was after the controls were lifted. Organic carbon (OC), organic molecular markers (e.g., levoglucosan, hopanes, polycyclic aromatic hydrocarbons), and secondary organic carbon (SOC) tracers were all significantly lower during the controlled period. After pollution controls ended, at Peking University, OC source contributions included gasoline and diesel engines (24%), coal combustion (6%), biomass burning (12.2%), vegetative detritus (2%), biogenic SOC (from isoprene, α-pinene, and β-caryophyllene; 7.1%), aromatic SOC (23%), and other sources not included in the model (25%). At Longgang after the controls ended, similar source contributions were observed: gasoline and diesel engines (23%), coal combustion (7%), biomass burning (17.7%), vegetative detritus (1%), biogenic SOC (from isoprene, α-pinene, and β-caryophyllene; 5.3%), aromatic SOC (13%), and other sources (33%). The contributions of the following sources were smaller during the pollution controls: biogenic SOC (by a factor of 10–16), aromatic SOC (4–12), coal combustion (1.5–6.8), and biomass burning (2.3–4.9). CMB model results and radiocarbon measurements both indicated that fossil carbon dominated over modern carbon, regardless of pollution controls. However, the CMB model needs further improvement to apportion contemporary carbon (i.e. biomass burning, biogenic SOC) in this region. This work defines the major contributors to carbonaceous PM2.5 in Shenzhen and demonstrates that control measures for primary emissions could significantly reduce secondary organic aerosol (SOA) formation.
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