The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol (SOA) formation experiments performed in Teflon chambers. A number of particle wall-loss correction methods have been proposed including the use of a size-independent loss rate constant, the ratio of suspended organic mass to that of a conserved tracer (e.g., sulfate seeds), and a size-dependent loss rate constant, etc.For complex experiments such as the chemical aging of SOA, the results of the SOA quantification analysis can be quite sensitive to the adopted correction method due to the evolution of the particle size distribution and the duration of these experiments.We evaluated the performance of several particle wallloss correction methods for aging experiments of α-pinene ozonolysis products. Determining the loss rates from seed loss periods is necessary for this system because it is not clear when chemical reactions have been completed. Results from the OA / sulfate ratio and the size-independent correction methods can be influenced significantly by the size dependence of the particle wall-loss process. Coagulation can also affect the particle size distribution, especially for particles with diameter less than 100 nm, thus introducing errors in the results of the wall-loss correction. The corresponding loss rate constants may vary from experiment to experiment, and even during a specific experiment. Friction between the Teflon chamber walls and non-conductive surfaces can significantly increase particle wall-loss rates and the chamber may require weeks to recover to its original condition. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments and the evaluation of corresponding particle wall-loss correction.
Abstract. In the present work, we performed chassis dynamometer experiments to investigate the emissions and secondary organic aerosol (SOA) formation potential of intermediate-volatility organic compounds (IVOCs) from an on-road Chinese gasoline vehicle. High IVOC emission factors (EFs) and distinct volatility distribution were recognized. The IVOC EFs for the China V vehicle ranged from 12.1 to 226.3 mg per kilogram fuel, with a median value of 83.7 mg per kilogram fuel, which was higher than that from US vehicles. Besides, a large discrepancy in volatility distribution and chemical composition of IVOCs from Chinese gasoline vehicle exhaust was discovered, with larger contributions of B14–B16 compounds (retention time bins corresponding to C14-C16 n-alkanes) and a higher percentage of n-alkanes. Further we investigated the possible reasons that influence the IVOC EFs and volatility distribution and found that fuel type, starting mode, operating cycles and acceleration rates did have an impact on the IVOC EF. When using E10 (ethanol volume ratio of 10 %, v/v) as fuel, the IVOC EF of the tested vehicle was lower than that using commercial China standard V fuel. The average IVOC-to-THC (total hydrocarbon) ratios for gasoline-fueled and E10-fueled gasoline vehicles were 0.07±0.01 and 0.11±0.02, respectively. Cold-start operation had higher IVOC EFs than hot-start operation. The China Light-Duty Vehicle Test Cycle (CLTC) produced 70 % higher IVOCs than those from the Worldwide Harmonized Light Vehicles Test Cycle (WLTC). We found that the tested vehicle emitted more IVOCs at lower acceleration rates, which leads to high EFs under CLTC. The only factor that may influence the volatility distribution and compound composition is the engine aftertreatment system, which has compound and volatility selectivity in exhaust purification. These distinct characteristics in EFs and volatility may result in higher SOA formation potential in China. Using published yield data and a surrogate equivalent method, we estimated SOA formation under different OA (organic aerosol) loading and NOx conditions. Results showed that under low- and high-NOx conditions at different OA loadings, IVOCs contributed more than 80 % of the predicted SOA. Furthermore, we built up a parameterization method to simply estimate the vehicular SOA based on our bottom-up measurement of VOCs (volatile organic compounds) and IVOCs, which would provide another dimension of information when considering the vehicular contribution to the ambient OA. Our results indicate that vehicular IVOCs contribute significantly to SOA, implying the importance of reducing IVOCs when making air pollution controlling policies in urban areas of China.
10The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol (SOA) formation experiments performed in Teflon chambers. A number of particle wall-loss correction methods have been proposed including the use of a size-independent loss rate constant, ratio of suspended organic mass to that of a conserved tracer (e.g., sulfate seeds), size-dependent loss rate constant, etc. For 15 complex experiments such as chemical aging of SOA, the results of the SOA quantification analysis can be quite sensitive to the adopted correction method due to the evolution of the particle size distribution and the duration of these experiments.We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Determining the loss rates from seed loss periods is 20 necessary for this system because it is not clear when chemistry is over. Results from the organic to sulfate ratio and the size-independent correction methods can be influenced significantly by the size-dependence of the particle wall-loss process. Coagulation can also affect the particle size distribution, especially for particles with diameter less than 100 nm, thus introducing errors in the results of the wall-loss correction. The corresponding loss rate constants may vary from 2 chamber walls and non-conductive surfaces can significantly increase particle wall-loss rates and the chamber may require weeks to recover to its original condition. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments and the evaluation of corresponding particle wall-loss correction.
A dual smog chamber system was used to quantify the formation rates of secondary organic and inorganic aerosol in an urban environment (Pittsburgh, US). Ambient air was introduced in both chambers, and HONO photolysis was used to produce hydroxyl radicals (OH) in the perturbed chamber. The second chamber was used as a reference. The production rate of secondary organic aerosol (SOA) under typical noon-time OH concentrations ranged from 0.2 to 0.8 μg m–3 h–1. The production rate of sulfate was approximately five times less than that of the SOA. Nucleation and growth of new particles were observed in the perturbation chamber. The produced SOA had a similar composition with the preexisting oxygenated ambient OA. The reacted amounts of the measured VOCs were able to explain 5–50% of the formed SOA in the perturbed chamber. Intermediate volatility organic compounds could be responsible for the rest. The oxygen to carbon ratio (O:C) in the perturbed chamber remained approximately the same during SOA production, while an increase was observed in the control chamber. A possible explanation could be the loss of less oxidized species to the chamber walls. After 2 h, the OA increased by 70% on average and the sulfate by 40%.
Abstract. Smog chamber experiments using ambient air as a starting point can improve our understanding of the evolution of atmospheric particulate matter at timescales longer than those achieved by traditional laboratory experiments. These types of studies can take place under more realistic environmental conditions addressing the interactions among multiple pollutants. The use of two identical smog chambers, with the first serving as the baseline chamber and the second as the perturbation chamber (in which addition or removal of pollutants, addition of oxidants, change in the relative humidity, etc.), can facilitate the interpretation of the results in such inherently complex experiments. The differences of the measurements in the two chambers can be used as the basis for the analysis of the corresponding chemical or physical processes of ambient air. A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers (1.5 m3 each). The two chambers are surrounded by UV lamps in a hexagonal arrangement yielding a total JNO2 of 0.1 min−1. The system can be easily disassembled and transported, enabling the study of various atmospheric environments. Moreover, it can be used with natural sunlight. The results of test experiments using ambient air as the starting point are discussed as examples of applications of this system.
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