Ground-level ozone (O3) pollution has received widespread attention because its rising trend and adverse ecological impacts. However, the extremely strong photochemical reactions of its precursor volatile organic compounds (VOCs) increase the difficulty of reducing VOCs emissions to alleviate O3. Here, we carried out a one-year comprehensive observation in two representative cities, Tianjin (TJ, Northern China) and Guangzhou (GZ, Southern China). By revealing the concentration characteristics of three different types of VOCs, i.e., initial VOCs without photochemical reaction (In-VOCs), consumed VOCs (C-VOCs), and measured VOCs after the reaction (M-VOCs), we elucidated the important role of C-VOCs in the formation of O3. Although the overall trends were similar in both cities, the average concentration level of VOCs in GZ was 8.2 ppbv higher than that in TJ, and the photochemical loss of VOCs was greater by 2.2 ppbv. In addition, various drivers affecting O3 generation from C-VOCs were specifically explored, and it was found that most alkenes of TJ were key substances for rapid O3 formation compared to aromatics of GZ. Meanwhile, favorable meteorological conditions such as high temperature (T > 31 °C in TJ, and T > 33 °C in GZ), low relative humidity (56% in TJ and 45% in GZ), and stable atmospheric environment (proper pressure and gentle wind speed) also contribute to the generation of O3. More importantly, we combined chemical kinetics and receptor model to quantify the three-type VOCs source contributions and assess the potential impact of C-VOCs sources on O3 production, thus proposing environmental abatement technologies corresponding to the three types of VOCs. The differences in the comparison results of the three-type VOCs highlight the need to reduce O3 pollution from C-VOCs sources, which provides insights for future clean air policies development.
Raloxifene (RXF) is a hormone-like medication used for treating postmenopausal osteoporosis and estrogen-dependent breast cancer, yet associated with bad low bioavailability due to poor solubility. This study was intended to develop cyclodextrin/chitosan nanoparticles (ccNPs) for oral delivery of RXF in order to enhance the oral bioavailability. RXF-loaded ccNPs (RXF-ccNPs) were prepared by cyclodextrin inclusion followed by complexation with chitosan. RXF-ccNPs were fully characterized by particle size, morphology and in vitro drug release. The oral delivery efficacy and transepithelial transport potential were evaluated by pharmacokinetics, in situ single-pass intestinal perfusion, cellular uptake and ex vivo imaging. The resulting RXF-ccNPs were around 165 nm in particle size with a narrow distribution. The oral bioavailability of RXF was enhanced by 2.6 folds through ccNPs compared to RXF suspensions in rats. It was shown that RXF-ccNPs could improve the intestinal permeability of RXF, increase the cellular uptake of RXF and facilitate its transport across the absorptive epithelia. The results indicate that our developed ccNPs based on sulfobutylether-β-cyclodextrin and oligochitosan are a promising vehicle to orally deliver poorly water-soluble drugs over and above RXF.
10 June 2023 in Frontiers of Environmental Science & Engineering
The mixing states of particulate amines with different chemical components are of great significance in studying the formation and evolution processes of amine-containing particles. In this work, the mixing states of single particles containing trimethylamine (TMA) and diethylamine (DEA) are investigated using a high-performance single-particle aerosol mass spectrometer located in Nanjing, China, in September 2019. TMA- and DEA-containing particles accounted for 22.8 % and 5.5 % of the total detected single particles, respectively. The particle count and abundance of the TMA-containing particles in the total particles notably increased with enhancement of ambient relative humidity (RH), while the DEA-containing particles showed no increase under a high RH. This result suggested the important role of RH in the formation of particulate TMA. Significant enrichments of secondary organic species, including 43C2H3O+, 26CN−, 42CNO−, 73C3H5O , and 89HC2O , were found in DEA-containing particles, indicating that DEA-containing particles were closely associated with the aging of secondary organics. The differential mass spectra of the DEA-containing particles showed a much higher abundance of nitrate and organic nitrogen species during the nighttime than during the daytime, which suggested that the nighttime production of particulate DEA might be associated with reactions of gaseous DEA with HNO3 and/or particulate nitrate. In the daytime, the decrease in DEA-containing particles was observed with the enrichment of oxalate and glyoxylate, which suggested a substantial impact of photochemistry on the aging process of DEA-containing particles. Furthermore, more than 80 % of TMA- and DEA-containing particles internally mixed with nitrate, while the abundance of sulfate was higher in the DEA-containing particles (79.3 %) than in the TMA-containing particles (55.3 %). This suggested that particulate DEA existed both as nitrate and sulfate aminium salts, while the particulate TMA primarily presented as nitrate aminium salt. The different mixing states of the TMA- and DEA-containing particles suggested their different formation processes and various influencing factors, which are difficult to investigate using bulk analysis. These results provide insights into the discriminated fates of organics during the evolution process in aerosols, which helps to illustrate the behavior of secondary organic aerosols.
The distribution of vanadium (V) in aerosols is commonly used to track ship exhaust emissions, yet the atmospheric abundance of V has been greatly reduced due to the implementation of a clean fuel policy. Recent research mainly discussed the chemical compositions of ship-related particles during specific events, yet few studies focus on the long-term changes of V in the atmosphere. In this study, a single-particle aerosol mass spectrometer was used to measure V-containing particles from 2020 to 2021 in Huangpu Port in Guangzhou, China. The long-term trend of the particle counts of V-containing particles declined annually, but the relative abundance of V-containing particles in the total single particles increased in summer due to the influence of ship emissions. Positive matrix factorization revealed that in June and July 2020, 35.7% of the V-containing particles were from ship emissions, followed by dust and industrial emissions. Furthermore, more than 80% of the V-containing particles were found mixing with sulfate and 60% of the V-containing particles were found mixing with nitrate, suggesting that the majority of the V-containing particles were secondary particles processed during the transport of ship emissions to urban areas. Compared with the small changes in the relative abundance of sulfate in the V-containing particles, the relative abundance of nitrate exhibited clear seasonal variations, with a high abundance in winter. This may have been due to the increased production of nitrate from high concentrations of precursors and a suitable chemical environment. For the first time, the long-term trends of V-containing particles in two years are investigated to demonstrate changes in their mixing states and sources after the clean fuel policy, and to suggest the cautious application of V as an indicator of ship emissions.
In this study, typical haze pollution influenced by biomass burning (BB) activities in Changsha in the autumn of 2024 was investigated through the mixing state and evolution process of BB particles via the real-time measurement of single-particle aerosol mass spectrometry (SPAMS). From the clean period to the haze period, the PM2.5 concentration increased from 25 μg·m−3 at 12:00 to 273 μg·m−3 at 21:00 on 12 October, and the proportion of total BB single particles in the total detected particles increased from 17.2% to 54%. This indicates that the rapid increase in PM2.5 concentration was accompanied by a concurrent increase in the contribution of particles originating from BB sources. The detected BB particles were classified into two types based on their mixing states and temporal variations: BB1 and BB2, which accounted for 71.7% and 28.3% of the total BB particles, respectively. The analysis of backward trajectories and fire spots suggested that BB1 particles originated from straw burning emissions at northern Changsha, while BB2 particles were primarily related to local nighttime cooking emissions in Changsha. In addition, a special type of K-containing single particles without K cluster ions was found closely associated with BB1 type particles, which were designated as secondarily processed BB particles (BB-sec). The BB-sec particles contained abundant sulfate and ammonium signals and showed lagged appearance after the peak of BB1-type particles, which was possibly due to the aging and formation of ammonium sulfate on the freshly emitted particles. In all, this study provides insights into understanding the substantial impact of BB sources on regional air quality during the crop harvest season and the appropriate disposal of crop straw, including conversion into high-efficiency fuel through secondary processing or clean energy via biological fermentation, which is of great significance for the mitigation of local haze pollution.