Secondary organic aerosol (SOA) contributes a significant fraction to aerosol mass and toxicity.Low-volatility organic vapors are critical intermediates connecting the oxidation of volatile organic compounds (VOCs) to SOA formation. However, the direct measurement of intermediate vapors poses a great challenge, further compounded by the difficulty of linking them to specific precursors from a cocktail of complex emission sources in the vast urbanized areas. Here, we present coordinated measurements of low-volatility oxidation products, termed oxygenated organic molecules (OOMs) in three most urbanized regions in China. With a newly-developed analysis methodology, we are able to assign these OOMs to their likely precursors and ultimately connect SOA formation to various VOCs. At all measurement locations, we find similar OOM
Intermediate volatility organic compound (IVOC) emissions from a large cargo vessel were characterized under realworld operating conditions using an on-board measurement system. Test ship fuel-based emission factors (EFs) of total IVOCs were determined for two fuel types and seven operating conditions. The average total IVOC EF was 1003 ± 581 mg•kg-fuel −1 , approximately 0.76 and 0.29 times the EFs of primary organic aerosol (POA) emissions from low-sulfur fuel (LSF, 0.38 wt % S) and high-sulfur fuel (HSF, 1.12 wt % S), respectively. The average total IVOC EF from LSF was 2.4 times that from HSF. The average IVOC EF under low engine load (15%) was 0.5−1.6 times higher than those under 36%−74% loads. An unresolved complex mixture (UCM) contributed 86.1 ± 1.9% of the total IVOC emissions. Ship secondary organic aerosol (SOA) production was estimated to be 546.5 ± 284.1 mg•kg-fuel −1 ; IVOCs contributed 98.9 ± 0.9% of the produced SOA on average. Fuel type was the dominant determinant of ship IVOC emissions, IVOC volatility distributions, and SOA production. The ship emitted more IVOC mass, produced higher proportions of volatile organic components, and produced more SOA mass when fueled with LSF than when fueled with HSF. When reducing ship POA emissions, more attention should be paid to commensurate control of ship SOA formation potential.
Although ambient PM2.5 has been linked to adverse health effects, the chemical constituents that cause harm are largely unclear. Few prior studies in a developing country have reported the health impacts of PM2.5 constituents. In this study, we examined the short-term association between PM2.5 constituents and emergency room visits in Shanghai, China. We measured daily concentrations of PM2.5, organic carbon (OC), elemental carbon (EC), and eight water-soluble ions between January 1, 2011 and December 31, 2012. We analyzed the data using overdispersed generalized linear Poisson models. During our study period, the mean daily average concentration of PM2.5 in Shanghai was 55 μg/m(3). Major contributors to PM2.5 mass included OC, EC, sulfate, nitrate, and ammonium. For a 1-day lag, an interquartile range increment in PM2.5 mass (36.47 μg/m(3)) corresponded to 0.57% [95% confidence interval (CI): 0.13%, 1.01%] increase of emergency room visits. In all the three models used, we found significant positive associations of emergency room visits with OC and EC. Our findings suggest that PM2.5 constituents from the combustion of fossil fuel (e.g., OC and EC) may have an appreciable influence on the health impact attributable to PM2.5.
During the COVID-19 lockdown period (from January 23 to February 29, 2020), ambient PM 2.5 concentrations in the Yangtze River Delta (YRD) region were observed to be much lower, while the maximum daily 8 h average (MDA8) O 3 concentrations became much higher compared to those before the lockdown (from January 1 to 22, 2020). Here, we show that emission reduction is the major driving force for the PM 2.5 change, contributing to a PM 2.5 decrease by 37% to 55% in the four YRD major cities (i.e., Shanghai, Hangzhou, Nanjing, and Hefei), but the MDA8 O 3 increase is driven by both emission reduction (29%–52%) and variation in meteorological conditions (17%– 49%). Among all pollutants, reduction in emissions mainly of primary PM contributes to a PM 2.5 decrease by 28% to 46%, and NOx emission reduction contributes 7% to 10%. Although NOx emission reduction dominates the MDA8 O 3 increase (38%–59%), volatile organic compounds (VOCs) emission reduction lead to a 5% to 9% MDA8 O 3 decrease. Increased O 3 promotes secondary aerosol formation and partially offsets the decrease of PM 2.5 caused by the primary PM emission reductions. The results demonstrate that more coordinated air pollution control strategies are needed in YRD.
Understanding the origin of fine particulate matter is essential to proposing proper strategies for heavy haze mitigation in Shanghai, China. In this study we used the Particulate Matter Source Apportionment Technology in Comprehensive Air Quality Model with Extensions to quantify the impacts of emissions on the concentrations of fine particulate matter (PM 2.5 ) and its important components in Shanghai during heavy haze episodes in late autumn (6-22 November 2010). The factors considered here are regions of Shanghai and its surrounding areas, long-range regional transport, and different local emission categories. The results indicate that industrial process is the dominant local contributor to total PM 2.5 mass in the whole city except that at the urban center vehicle emission contributes slightly more. In addition, industrial process and vehicle emission are the major local contributors for nitrate in Shanghai, although at urban core the contribution from vehicle emission is remarkably larger. Generally, both local contribution and regional transport contribution could dominate a severe haze event in late autumn. However, the dominant contributor could either be local emission or regional transport, usually depending on the meteorological conditions. Therefore, particular attentions should be paid to the emission control in the upwind adjacent provinces, as well as in local areas, for developing effective strategies to reduce PM 2.5 pollution in Shanghai.
Molecular markers in ambient organic aerosol (OA) provide highly specific source information. Their traditional quantification is based on offline analysis of filter samples, and the coarse time resolution and labor-intensive nature hugely limit the utility of the tracer data. In this study, hourly organic molecular markers in fine particulate matter were measured using a recently commercialized thermal desorption aerosol gas chromatography− mass spectrometry (TAG) technique at an urban location in Shanghai, China during a three-week campaign from 9 November to 3 December, 2018. Selected primary OA molecular markers, including anhydrosugars, fatty acids, aromatic acids, and polycyclic aromatic hydrocarbons (PAHs), were examined in detail. Their diurnal variations showed characteristic features representing the corresponding emission source activities. For example, stearic acid showed a clear peak around 7 pm, in accordance with the enhanced cooking activities during mealtime. Diagnostic ratios of related makers of different reactivities provided unique information in uncovering the source information and tracking evolution of the OA in the atmosphere, for example, ratios of levoglucosan to its isomers and K + identified crop residue burning as the major form of biomass burning (BB). Ratios of unsaturated and saturated fatty acids gave unambiguous indication of atmospheric degradation of unsaturated fatty acids after emissions. Oleic acid to stearic acid ratios in ambient data (0.83 ± 0.54) were lower than those in the source profiles (1.2−6.5). Furthermore, the oleic acid to stearic acid ratio was found to be highly correlated with O/C ratios (R p : −0.66), suggesting the possible utility of oleic acid as a model compound to examine the heterogeneous reaction of cooking-related OA. PAH ratio−ratio plots helped identify varying influences of major combustion sources associated with air masses of different origins, revealing that BB and coal combustion were dominant under the influence of long-range transport air mass, while vehicle emissions were dominant under local/median-range air mass influence. This study demonstrated the utility of high time-resolution organic markers in capturing the dynamic change of source emissions and atmospheric aging, providing observational evidence to support their use in source apportionment.
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