An extensive set of primary and secondary pollutants was measured at a ground site in a remote location in the Yellow River Delta, China during the Ozone Photochemistry and Export from China Experiment (OPECE) from March to April 2018. The measurements include volatile organic compounds (VOCs), peroxyacyl nitrates (PANs), ozone (O3), particulate species, nitrogen oxides (NOx), and SO2. Observed VOC mixing ratios were comparable to those measured in heavily polluted cities in the U.S. and China. The VOC source signatures suggest a strong influence from Oil and Natural Gas (O&NG) emissions with potentially large contributions from Liquified Petroleum Gas (LPG) sources as well. Consistently elevated concentrations of O3, PAN, and its rarely measured homologs peroxybenzoylic nitric anhydride (PBzN) and peroxyacrylic nitric anhydride (APAN) at the OPECE site indicate complex photochemistry in a heterogeneous VOC environment. Diagnostic 0‐D box model simulations are used to investigate the budgets of ROx(OH + HO2 + RO2), and the rate and efficiency of O3production. Model sensitivity calculations indicate that O3production at OPECE site is VOC limited in spring. This suggests that reduction in VOCs should be a priority for reducing O3, where production and fugitive emissions from O&NG provide an attractive target. While initial reductions in NOxmight increase O3production, reduction of NOxalong with VOCs will be a necessary step to achieve long‐term ozone reduction.
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Abstract High ozone concentrations have become the major summertime air quality problem in China. Extensive in situ observations are deployed for developing strategies to effectively control the emissions of ozone precursors, that is, nitrogen oxides (NOX = NO + NO2) and volatile organic compounds (VOCs). The modeling analysis of in situ observations often makes uses of the dependence of ozone peak concentration on NOXand VOC emissions, because ozone observations are among the most widely available air quality measurements. To extract more information from regulatory ozone observations, we extend the ozone‐precursor relationship to ozone peak time in this study. We find that the sensitivities of ozone peak time and concentration are complementary for regions with large anthropogenic emissions such as China. The ozone peak time is sensitive to both VOC and NOXemissions, and the sensitivity is nearly linear in the transition regime of ozone production compared to the changing ozone peak concentration sensitivity in this regime, making the diagnostics of ozone peak time particularly valuable. The extended ozone‐precursor relationships can be readily applied to understand the effects on ozone by emission changes of NOXand VOC and to assess potential biases of NOXand VOC emission inventories. These observation constraints based on regulatory ozone observations can complement the other measurement and modeling analysis methods nicely. Furthermore, we suggest that the ozone peak time sensitivity we discussed here to be used as a model evaluation measure before the empirical kinetic modeling approach (EKMA) diagram is applied to understand the effectiveness of emission control on ozone concentrations.
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Abstract Ammonia control has received increasing attention as a measure to decrease particulate concentrations. Modeling analysis of observation data from central China over the period of September 2015 to August 2016 shows clear asymmetric responses of particulate pH and mass to ammonia emissions. With a change of ±80% of NH
x (NH3+ NH4+), the corresponding ΔpH are +0.5 and −3.0, respectively, and the corresponding particulate NH4+changes are +2.62% and −61.8%, respectively. This asymmetry implies that there is a Critical Total Ammonia Concentration, above which particulate pH and mass are insensitive to ammonia control. Analysis of the observation data suggests that the Critical Total Ammonia Concentration is −25%. The estimated cost for an NHx reduction of 25% is $140 – 320 million for Hubei province, which is the initial cost barrier before ammonia control can effectively affect particulate pH and mass in central China. This cost barrier will increase as NOx and SO2emissions decrease. -
Abstract Background The spatiotemporal variation of observed trace gases (NO 2 , SO 2 , O 3 ) and particulate matter (PM 2.5 , PM 10 ) were investigated over cities of Yangtze River Delta (YRD) region including Nanjing, Hefei, Shanghai and Hangzhou. Furthermore, the characteristics of different pollution episodes, i.e., haze events (visibility < 7 km, relative humidity < 80%, and PM 2.5 > 40 µg/m 3 ) and complex pollution episodes (PM 2.5 > 35 µg/m 3 and O 3 > 160 µg/m 3 ) were studied over the cities of the YRD region. The impact of China clean air action plan on concentration of aerosols and trace gases is examined. The impacts of trans-boundary pollution and different meteorological conditions were also examined. Results The highest annual mean concentrations of PM 2.5 , PM 10 , NO 2 and O 3 were found for 2019 over all the cities. The annual mean concentrations of PM 2.5 , PM 10 , and NO 2 showed continuous declines from 2019 to 2021 due to emission control measures and implementation of the Clean Air Action plan over all the cities of the YRD region. The annual mean O 3 levels showed a decline in 2020 over all the cities of YRD region, which is unprecedented since the beginning of the China’s National environmental monitoring program since 2013. However, a slight increase in annual O 3 was observed in 2021. The highest overall means of PM 2.5 , PM 10 , SO 2 , and NO 2 were observed over Hefei, whereas the highest O 3 levels were found in Nanjing. Despite the strict control measures, PM 2.5 and PM 10 concentrations exceeded the Grade-1 National Ambient Air Quality Standards (NAAQS) and WHO (World Health Organization) guidelines over all the cities of the YRD region. The number of haze days was higher in Hefei and Nanjing, whereas the complex pollution episodes or concurrent occurrence of O 3 and PM 2.5 pollution days were higher in Hangzhou and Shanghai. The in situ data for SO 2 and NO 2 showed strong correlation with Tropospheric Monitoring Instrument (TROPOMI) satellite data. Conclusions Despite the observed reductions in primary pollutants concentrations, the secondary pollutants formation is still a concern for major metropolises. The increase in temperature and lower relative humidity favors the accumulation of O 3 , while low temperature, low wind speeds and lower relative humidity favor the accumulation of primary pollutants. This study depicts different air pollution problems for different cities inside a region. Therefore, there is a dire need to continuous monitoring and analysis of air quality parameters and design city-specific policies and action plans to effectively deal with the metropolitan pollution.more » « less
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The continued development of the automotive industry has led to a rapid increase in the amount of waste rubber tires, the problem of “black pollution” has become more serious but is often ignored. In this study, the emission characteristics, health risks, and environmental effects of volatile organic compounds (VOCs) from a typical, recycled rubber plant were studied. A total of 15 samples were collected by summa canisters, and 100 VOC species were detected by the GC/MS-FID system. In this study, the total VOCs (TVOCs) concentration ranged from 1000 ± 99 to 19,700 ± 19,000 µg/m3, aromatics and alkanes were the predominant components, and m/p-xylene (14.63 ± 4.07%–48.87 ± 3.20%) could be possibly regarded as a VOCs emission marker. We also found that specific similarities and differences in VOCs emission characteristics in each process were affected by raw materials, production conditions, and process equipment. The assessment of health risks showed that devulcanizing and cooling had both non-carcinogenic and carcinogenic risks, yarding had carcinogenic risks, and open training and refining had potential carcinogenic risks. Moreover, m/p-xylene and benzene were the main non-carcinogenic species, while benzene, ethylbenzene, and carbon tetrachloride were the dominant risk compounds. In the evaluation results of LOH, m/p-xylene (25.26–67.87%) was identified as the most key individual species and should be prioritized for control. In conclusion, the research results will provide the necessary reference to standardize the measurement method of the VOCs source component spectrum and build a localized source component spectrum.more » « less
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Abstract A catastrophic heatwave struck North America (NA) in the summer of 2021, the underlying cause of which currently remains unclear. The reanalysis data (1980–2021) is analyzed to elucidate the mechanism modulating the summer heatwaves. We find the heatwaves over western NA tend to occur concurrently with quasi-barotropic ridges (QBTRs). The 2021 record-breaking heatwave, in particular, coincides with an extended eight-day QBTR event. The frequency of QBTRs is modulated by large-scale forcing. During the period of 1980–2000, it is correlated with the Arctic Oscillation. After 2000, however, the QBTR frequency is highly associated with sea ice variations. Specifically, the negative sea ice anomalies in the Chukchi Sea are usually associated with stronger net surface shortwave radiation and low cloud cover, triggering upward motion and a low-pressure center in the low- and mid-troposphere. The low pressure strengthens a stationary wave response, concomitant with two alternately high- and low-pressure centers, inducing more frequent QBTRs over western NA. These findings indicate that further Arctic sea ice loss under a warming climate will likely lead to more devastating heatwaves over western NA.more » « less
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China has been experiencing severe ozone pollution problems in recent years. While a number of studies have focused on the ozone-pollution-prone regions such as the North China Plain, Yangtze River Delta, and Pearl River Delta regions, few studies have investigated the mechanisms modulating the interannual variability of ozone concentrations in Shandong Province, where a large population is located and is often subject to ozone pollution. By utilizing both the reanalysis dataset and regional numerical model (WRF-CMAQ), we delve into the potential governing mechanisms of ozone pollution in Shandong Province—especially over the major port city of Qingdao—during summer 2014–2019. During this period, ozone pollution in Qingdao exceeded the tier II standard of the Chinese National Ambient Air Quality (GB 3095-2012) for 75 days. From the perspective of meteorology, the high-pressure ridge over Baikal Lake and to its northeast, which leads to a relatively low humidity and sufficient sunlight, is the most critical weather system inducing high-ozone events in Qingdao. In terms of emissions, biogenic emissions contribute to ozone enhancement close to 10 ppb in the west and north of Shandong Province. Numerical experiments show that the local impact of biogenic emissions on ozone production in Shandong Province is relatively small, whereas biogenic emissions on the southern flank of Shandong Province enhance ozone production and further transport northeastward, resulting in an increase in ozone concentrations over Shandong Province. For the port city of Qingdao, ship emissions increase ozone concentrations when sea breezes (easterlies) prevail over Qingdao, with the 95th percentile reaching 8.7 ppb. The findings in this study have important implications for future ozone pollution in Shandong Province, as well as the northern and coastal areas in China.more » « less