New mechanism for the participation of aromatic oxidation products in atmospheric nucleation.

Oxygenated organic molecules (OOMs) are recognized as important precursors for new particle formation (NPF) in the urban atmosphere. The paper theoretically studied the formation of OOMs by styrene oxidation processes initiated by OH radicals, focusing on the OOMs nucleation mechanism. The results found that in the presence of an H2SO4 molecule, lowly oxygenated organic molecules containing a benzene ring (LOMBs) can form stable clusters and grow to the scale of a critical nucleus through pi-pi stacking and OH hydrogen bonding. In addition, LOMBs are more readily generated in a styrene-oxidized system in the presence/absence of NOx than highly oxygenated organic molecules (HOMs). The reaction of OH radicals with other aromatics containing a branched chain on the benzene ring produces LOMBs to varying degrees, with pi-pi stacking playing an essential role. This result suggests that, in the presence of H2SO4 molecules, LOMBs may play a more significant role in promoting nucleation than HOMs. Our findings serve as a pivotal foundation for future investigations into the oxidation and nucleation processes of diverse aromatics in urban environments.

A neglected pathway for the accretion products formation in the atmosphere.

Highly oxygenated organic molecules (HOM) formed by the autoxidation of α-pinene initiated by OH radicals play an important role in new particle formation. It is believed that the accretion products, ROOR´, formed by the self- and cross-reaction of peroxy radicals (RO2 + R'O2 reactions), have extremely low volatility and are more likely to participate in nucleation. However, the mechanism of ROOR´ formation has not been fully demonstrated by experiment or theoretical calculation. Herein, we propose a novel mechanism of RO2 reacting with α-pinene (RO2 + α-pinene reactions) that have much lower potential barriers and larger rate constants than the reaction of RO2 with R'O2, which explains the ROOR´ formation found in the mass spectrometry experiments. The ROOR´ resulting from the reaction of RO2 with α-pinene can produce HOM dimers and trimers with a higher oxygen-to­carbon (O/C) ratio through a autoxidation chain. We also demonstrated that the presence of NOx and HO2 radical will reduce the RO2 concentration, but cannot completely inhibit the formation of HOM monomers and ROOR´. Even if one or both of RO2 radicals are acyl peroxy radicals (RC(O)O2), the potential barriers of the reactions between RC(O)O2 and α-pinene (RC(O)O2 + α-pinene reactions) are lower than that of RO2 reacting with RC(O)O2 (RO2 + RC(O)O2 reactions) or RC(O)O2 self-reactions (RC(O)O2 + RC(O)O2 reactions). The current work revealed, for the first time, a mechanism of RO2/RC(O)O2 reacting with α-pinene in the atmosphere, which provides new insight into the atmospheric chemistry of accretion products as SOA precursors.

Photocatalytic concrete for degrading organic dyes in water.

Since the advent of photocatalytic degradation technology, it has brought new vitality to the environmental governance and the response to the energy crisis. Photocatalysts harvest optical energy to drive chemical reactions, which means people can use solar energy to complete some resource-consuming activities by photocatalysts, such as environmental governance. In recent years, researchers have tried to combine photocatalyst TiO2 with building materials to purify urban air and obtained good results. One of the important functions of photocatalysts is to degrade organic pollutants in water through light energy, but this technology has not been reported in the practical application areas. To extend this technology to practical application areas, photocatalytic concrete for degrading pollutants in waters was proposed and demonstrated for the first time in this paper. The photocatalytic concrete proposed based on the K-g-C3N4 shows a strong ability to degrade the organic dyes. According to the experiment results, the angle of light source plays an important role in the process of photocatalytic degradation, while waters with pH value of 6.5-8.5 hardly influenced the degradation of organic dyes. When the angle of light source is advantageous for photocatalytic concrete to absorb more visible light, more organic dyes will be degraded by photocatalytic concrete. The degradation rate of methylene blue could reach about 80% in ½ hour under desirable conditions and is satisfied compared with that of reported works. This study implicates that photocatalytic concrete can effectively degrade organic dyes in water. The influences of changes in the water environment hardly affect the degradation of organic pollutants, which means photocatalytic concrete can be widely used in green infrastructures to achieve urban sewage treatment.

Effects of air pollutant emission on the prevalence of respiratory and circulatory system diseases in Linyi, China.

As a typical industrial city, Linyi has suffered severe atmospheric pollution in recent years. Meanwhile, a high incidence of respiratory and circulatory diseases has been observed in Linyi. The relationship between air pollutants and the prevalence of respiratory and circulatory system diseases in Linyi is still unclear, and therefore, there is an urgent need to assess the human health risks associated with air pollutants. In this study, the number of outpatient visits and spatial distribution of respiratory and circulatory diseases were first investigated. To clarify the correlation between diseases and air pollutant emissions, the residential intake fraction (IF) of air pollutants was calculated. The results showed that circulatory and respiratory diseases accounted for 62.32% of the total causes of death in 2015. The incidence of respiratory diseases was high in the winter, and outpatient visits were observed for more males (60.9%) than females (39.1%). The spatial distribution suggested that outpatient visits for respiratory and circulatory diseases were concentrated in the main urban area of Linyi, including the Hedong District, Lanshan District, and Luozhuang District, and especially at the junction of these three areas. After calculating the IF combined with the characteristics of pollution sources, meteorological conditions, and population data, a high IF value was concentrated in urban and suburban areas, which was consistent with the high incidence of diseases. Moreover, high R values and a significant correlation (R > 0.6, p < 0.05) between outpatient visits and residential IF of air pollutants imply similar spatial distributions of outpatient visits and IF value of residents. The spatial similarity of air pollution and outpatient visits suggested that future air pollution control policies should better reflect the health risks of spatial hotspots. This study can provide a potentially important reference for environmental management and air pollution-related health interventions.

Model analysis of meteorology and emission impacts on springtime surface ozone in Shandong.

Air quality observations showed that surface ozone (O3) concentrations over Shandong increased significantly in springtime in recent years, especially 2017. The observed 90th percentile of hourly O3 concentrations (O3-h_90) in May increased from 148.4 µg/m3 in 2016 to 176.2 µg/m3 in 2017. To investigate the reasons of significant increase of O3 in spring of 2017, seven sensitivity cases were performed with the RAMS-CMAQ modeling system to identify the impacts of meteorological conditions (M) and emissions (E) on O3 concentrations in May of Shandong during the time period 2016-2018. The regional O3-h_90 in May of Shandong were 103.0, 120.3 and 86.3 µg/m3 in 2016, 2017 and 2018, respectively. It was found that the positive effects from favorable meteorology were the dominant reasons that resulted in the high O3 concentration in May 2017. When compared to 2017 standard simulation (17E17M), the differences of meteorological conditions led to the decrease of 17.5 and 33.8 µg/m3 in regional O3-h_90 of May in 2016 (17E16M) and 2018(17E18M), while small changes (0.6 and - 0.3 µg/m3) appeared in that of May 2016 (16E17M) and 2018(18E17M) due to emission differences. Since there were few differences in the wind speeds of May between three years, the higher temperature and lower relative humidity significantly contributed to O3 formation in May 2017 compared to May of 2016 and 2018. Besides, the amount of cloud fraction (CF), which has an indirect influence on the surface temperature and photochemical production of ozone by its impacts on the insolation, was the least in May 2017 compared to that in May 2016 and 2018 over Shandong. The distributions of changes in CF had obvious negative correlations with that of O3 vertical column concentrations and temperature. Thus, the fewer cloud fraction may play a key role in O3 formation of May 2017.

[Impact of Pollutant Emission Reduction on Air Quality During the COVID-19 Pandemic Control in Early 2020 Based on RAMS-CMAQ].

In this work, the relationships between air quality and pollutant emissions were investigated during the COVID-19 pandemic in Shandong Province. During the quarantine period (from January 24 to February 7, 2020), the concentrations of atmospheric pollutants decreased significantly relative to the period before controls were imposed (from January 15 to 23, 2020). Specifically, except for an increase in the concentration of O3, concentrations of PM10, PM2.5, NO2, SO2, and CO decreased for 72.6 µg·m-3 (45.86%), 47.4 µg·m-3(41.24%), 25.6 µg·m-3 (58.00%), 3.0 µg·m-3 (17.71%), and 0.5 mg·m-3 (31.40%), respectively. RAMS-CMAQ simulation showed that meteorological diffusion had an essential role in improving air quality. Influenced by meteorological factors, emissions of PM10, PM2.5, NO2, SO2, and CO were reduced 26.04%, 33.03%, 28.35%, 43.27%, and 23.29%, respectively. Furthermore, the concentrations of PM10, PM2.5, NO2, SO2, and CO were reduced by 19.82%, 8.21%, 29.65%, -25.56%, and 8.12%, respectively, due to pollution emissions reductions during the quarantine period. O3 concentrations increased by 20.51% during quarantine, caused by both meteorological factors (10.47%) and human activities (10.04%). These results indicate that primary pollutants were more sensitive to emissions reductions; however, secondary pollutants demonstrated a lagged response the emissions reduction and were significantly affected by meteorological factors. The linear relationship between ozone and the emissions reduction was not significant, and was inverse overall. Further investigation are now required on the impact of emissions reduction on ozone pollution control.

[Characteristics and Sources Apportionment of Fine Particulate Matter in a Typical Coastal City During the Heating Period].

To clarify the pollution characteristics and sources of PM2.5 in Weihai during the heating period, PM2.5 samples from ambient air were collected at three routine air quality monitoring sites from January to March 2018. The OC, EC, water-soluble ions, and elements in PM2.5 were analyzed, and the sources of PM2.5 were identified using the PMF model. The results showed that the average daily mass concentration of PM2.5 was (33.80±22.45) µg·m-3, and the NO3-, NH4+, SO42-, OC, and EC were the main components of PM2.5. As a coastal city, the Cl- ratio was relatively high in PM2.5. Meanwhile, the compositions of PM2.5 were affected by the emission of pollutants with local industrial characteristics. Both NO3-/SO42- and OC/EC showed that mobile sources had a high contribution during the heating period. The acid-base ions in water-soluble ions showed that PM2.5 is weakly alkaline, and NH4+ is excessive. NH4+ mainly existed in the form of NH4NO3 and (NH4)2SO4. During the polluted period, the concentration of secondary pollutants significantly increased, and the mass concentrations of NH4+, NO3-, SO42-, OC, and EC were 4.21, 5.27, 3.23, 2.02, and 1.81 times that of the cleaning period, respectively. The PMF model showed that secondary aerosols were the major source of PM2.5, accounting for 32.4%-36.0% of PM2.5. The contributions of vehicle exhaust, coal combustion, biomass burning, and dust were 15.6%-18.9%, 12.1%-17.8%, 9.0%-10.4%, and 8.6%-11.3%, respectively, while the contributions of process emission (2.1%-8.3%), non-road mobile sources (2.4%-3.7%), and sea salt (3.5%-5.6%) were less.

Pollution characteristics of bioaerosols in PM2.5 during the winter heating season in a coastal city of northern China.

Frequent heavy air pollution occurred during the winter heating season of northern China. In this study, PM2.5 (particles with an aerodynamic diameter less than 2.5 µm) was collected from a coastal city of China during the winter heating season from January 1 to March 31, 2018, and the soluble ions, organic carbon (OC), elemental carbon (EC), bacterial, endotoxin, and fungal concentration in PM2.5 were analyzed. During the winter heating season, PM2.5 and bioaerosols increased on polluted days, and the secondary inorganic ions, including NO3-, NH4+, and SO42-, increased significantly. Meteorological factors, such as wind direction and wind speed, had major impacts on the distributions of PM2.5 and bioaerosols. Pollutant concentration was high when there was a westerly wind with the speed of 3-6 m/s from inland area. Using the air mass backward trajectories and principal component analysis, we elucidate the potential origins of bioaerosol in PM2.5. The backward trajectory suggested that air mass for polluted samples (PM2.5 > 75 µg/m3) commonly originated from continent (9.62%), whereas air masses for clean samples (PM2.5 < 35 µg/m3) were mainly from marine (56.73%). The interregional transport of pollutants from continental area contributed most to PM2.5. Principal component analysis of the water-soluble ions and bioaerosol indicated that air pollution of the coastal city was greatly affected by coal combustion, biomass burning, and regional transmission of high-intensity pollutants from continent. Among that, interregional transport, biomass burning, and dust from soil and plants were main sources of bioaerosol. Our findings provide important insights into the origins and characteristics of bioaerosol in PM2.5 during the winter heating season of the coastal city in northern China.

Effects of aerosol pollution on PM2.5-associated bacteria in typical inland and coastal cities of northern China during the winter heating season.

Frequent heavy aerosol pollution occurs during the winter heating season in northern China. Here, we characterized the airborne bacterial community structure and concentration, during typical pollution episodes that occurred during the winter heating season of 2017-2018 in Jinan and Weihai. During this heating season, five and four heavy pollution episodes were observed in Jinan and Weihai, respectively. Compared with December and January, pollution episodes in March were significantly affected by sand dust events. Higher Bacillales were identified in the March samples from Jinan, indicating that sand dust influences bacterial communities. During similar pollution episodes, air pollution in the coastal city of Weihai was lower than the inland city of Jinan. The predominant bacteria included Staphylococcus, Cyanobacteria, Lactobacillus, Deinococcus, Enbydrobacter, Ralstonia, Bacillus, Comamonas, and Sphingomonas. These predominant bacteria are mainly from Proteobacteria, Firmicutes, Cyanobacteria, Actinobacteria, and Bacteroidetes phyla. Bacterial concentration showed significant variation with increased airborne pollutants. The highest concentration appeared during moderate pollution (up to 106 cells/m3), whereas bacterial concentration decreased during heavy and severe pollution (105 cells/m3), which may be related to toxic effects of high pollutant concentrations during heavy or severe pollution. Community structure variation indicated that Cyanobacterial genera were dominant in clean or slight pollution. With increased PM2.5, Staphylococcus increased and became the most abundant bacteria in moderate pollution (up to 40%). During heavy or severe pollution, bacteria that are adaptable to harsh or extreme environments predominate, such as Deinococcus and Bacillus. In the assessment of health risks from air pollution, the bioaerosols risks must consider. Additionally, although most microbial genera are similar between the two cities, there are important differences associated with pollution level. During air pollution regulation in different regions with varied geographical and climatic conditions, bioaerosol pollution difference is an unignored factor.

Measurement of hydrogen peroxide and organic hydroperoxide concentrations during autumn in Beijing, China.

Gaseous peroxides play important roles in atmospheric chemistry. To understand the pathways of the formation and removal of peroxides, atmospheric peroxide concentrations and their controlling factors were measured from 7:00 to 20:00 in September, October, and November 2013 at a heavily trafficked residential site in Beijing, China, with average concentrations of hydrogen peroxide (H2O2) and methyl hydroperoxide (MHP) at 0.55ppb and 0.063ppb, respectively. H2O2 concentrations were higher in the afternoon and lower in the morning and evening, while MHP concentrations did not exhibit a regular diurnal pattern. Both H2O2 and MHP concentrations increased at dusk in most cases. Both peroxides displayed monthly variations with higher concentrations in September. These results suggested that photochemical activity was the main controlling factor on variations of H2O2 concentrations during the measurement period. Increasing concentrations of volatile organic compounds emitted by motor vehicles were important contributors to H2O2 and MHP enrichment. High levels of H2O2 and MHP concentrations which occurred during the measurement period probably resulted from the transport of a polluted air mass with high water vapor content passing over the Bohai Bay, China.