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Seasonal variation and deposition of atmospheric organophosphate esters in the coastal region of Shanghai, China
2022
Ma, Yuxin | Luo, Yuchen | Zhu, Jincai | Zhang, Jinghua | Gao, Guoping | Mi, Wenying | Xie, Zhiyong | Lohmann, Rainer
The coastal megacity Shanghai is located in the center of the Yangtze River Delta, a dominant flame retardants (FRs) production region in China, especially for organophosphate esters (OPEs). This prompted us to investigate occurrence and seasonal changes of atmospheric OPEs in Shanghai, as well as to evaluate their sources, environmental behavior and fate as a case study for global coastal regions. Atmospheric gas and particle phase OPEs were weekly collected at two coastal sites - the emerging town Lingang New Area (LGNA), and the chemical-industry zone Jinshan Area (JSA) from July 2016–June 2017. Total atmospheric concentrations of the observed OPEs were significantly higher in JSA (median of 1800 pg m⁻³) than LGNA (median of 580 pg m⁻³). Tris(1-chloro-2-propyl) phosphate (TCPP) was the most abundant compound, and the proportion of three chlorinated OPEs were higher in the particle phase (55%) than in the gas phase (39%). The year-round median contribution of particle phase OPEs was 33%, which changed strongly with seasons, accounting for 10% in summer in contrast to 62% in winter. Gas and particle phase OPEs in JSA exhibited significant correlations with inverse of temperature, respectively, indicating the importance of local/secondary volatilization sources. The estimated fluxes of gaseous absorption were almost 2 orders of magnitude higher than those of particle phase deposition, which could act as sources of organic phosphorus to coastal and open ocean waters.
显示更多 [+] 显示较少 [-]An ICT-based fluorescent probe with a large Stokes shift for measuring hydrazine in biological and water samples
2020
Zhu, Meiqing | Xu, Yimin | Sang, Linfeng | Zhao, Zongyuan | Wang, Lijun | Wu, Xiaoqin | Fan, Fugang | Wang, Yi | Li, Hui
As a strong reductant and highly active alkali, hydrazine (N2H4) has been widely used in chemical industry, pharmaceutical manufacturing and agricultural production. However, its high acute toxicity poses a threat to ecosystem and human health. In the present study, a ratiometric fluorescent probe for the detection of N2H4 was designed, utilizing dicyanoisophorone as the fluorescent group and 4-bromobutyryl moiety as the recognition site. 4-(2-(3-(dicyanomethylene)-5,5-dimethylcyclohex-1-enyl) phenyl 4-brobutanoate (DDPB) was readily synthesized and could specially sense N2H4 via an intramolecular charge transfer (ICT) pathway. The cyclization cleavage reaction of N2H4 with a 4-bromobutyryl group released phenolic hydroxyl group and reversed the ICT process between hydroxy group and fluorophore, turning on the fluorescence in the DDPB-N2H4 complexes. DDPB exhibits a low cytotoxicity, reasonable cell permeability, a large Stokes shift (186 nm) and a low detection limit (86.3 nM). The quantitative determination of environmental water systems and the visualization fluorescence of DDPB test strips provides a strong evidence for the applications of DDPB. In addition, DDPB is suitable for the fluorescence imaging of exogenous N2H4 in HeLa cells and zebrafish.
显示更多 [+] 显示较少 [-]New insight of ozone pollution impact from flare emissions of chemical plant start-up operations
2019
Ge, Sijie | Zhang, Jian | Wang, Sujing | Xu, Qiang | Ho, Thomas
Flaring is a common and necessary operation for chemical industries, which is designed to manage dangerous process overpressure scenarios or to release and destroy off-spec products during chemical plant upsets or turnarounds. However, excessive flaring can emit large quantities of VOCs and NOx into the atmosphere, which will cause transient and localized ozone pollution events in the presence of sunlight. The objective of this study was to quantify the impact to regional air-quality due to flare emissions from chemical plant start-up operations through the coupling of dynamic process simulations via Aspen Plus and air-quality simulations via CAMx. Simulation results from case studies have indicated that the corresponding ozone increments can vary significantly from 0.2 ppb to 17.8 ppb under different temporal and spatial factors, including the start-up starting hour, starting day, and plant location. Additional ozone sensitivity simulations have also indicated that the corresponding ozone increments are higher when the plant is located in a VOC-limited area than that in a NOx-limited area. The results from this study have delivered a cost-effective air-quality control practice for plant start-ups with a minimum air-quality impact through selecting the optimal starting time within the allowable ranges. The practice has significant potential to benefit all stakeholders, including environmental agencies, chemical industries, and local communities.
显示更多 [+] 显示较少 [-]Levels and distribution of polybrominated diphenyl ethers (PBDEs) in the freshwater environment surrounding a PBDE manufacturing plant in China
2009
Xu, Jie | Gao, Zishen | Xian, Qiming | Yu, Hongxia | Feng, Jianfang
Polybrominated diphenyl ethers (PBDEs) were determined in muscle, liver and eggs of freshwater fishes and surface sediments from the Nongkang River in Jinhu, Jiangsu Province, China. The present study is the first to report PBDE concentrations in the freshwater environment surrounding a PBDE manufacturing plant in China. The concentrations of 13 PBDE congeners in muscle, liver and eggs of freshwater fishes ranged from <LOD to 130, <LOD to 252 and <LOD to 33.3 ng/g lipid wt, respectively, while the concentrations of 13 PBDE congeners in surface sediments from sewage outfall, upstream and downstream of the river were 52, 9.2, 7.1 ng/g organic carbon wt, respectively. Contamination by PBDEs in this area was not serious when compared with other regions of the world. A relatively high proportion of BDE-183 was found, consistent with the octa-BDE technical mixtures from the manufacturing plant by the side of the river. The first study to report concentrations of PBDEs in the freshwater environment surrounding a PBDE manufacturing plant in China.
显示更多 [+] 显示较少 [-]Mitigation of hazardous toluene via ozone-catalyzed oxidation using MnOx/Sawdust biochar catalyst
2022
Cha, Jin Sun | Kim, Young-Min | Lee, Im Hack | Choi, Yong Jun | Rhee, Gwang Hoon | Song, Hocheol | Jeon, Byong-Hun | Lam, Su Shiung | Khan, Moonis Ali | Andrew Lin, Kun-Yi | Chen, Wei-Hsin | Park, Young-Kwon
This study investigated catalytic ozone oxidation using a sawdust char (SDW) catalyst to remove hazardous toluene emitted from the chemical industry. The catalyst properties were analyzed by proximate, ultimate, nitrogen adsorption-desorption isotherms, Fourier-transform infrared, and X-ray photoelectron spectroscopy analyses. In addition, hydrogen-temperature programmed reduction experiments were conducted to analyze the catalyst properties. The specific area and formation of micropores of SDC were improved by applying KOH treatment. MnOx/SDC-K3 exhibited a higher toluene removal efficiency of 89.7% after 100 min than MnOx supported on activated carbon (MnOx/AC) with a removal efficiency of 6.6%. The higher (Oₐdₛ (adsorbed oxygen)+Oᵥ(vacancy oxygen))/OL (lattice oxygen) and Mn³⁺/Mn⁴⁺ ratios of MnOx/SDC-K3 than those of MnOx/AC seemed to be important for the catalytic oxidation of toluene.
显示更多 [+] 显示较少 [-]Reconstructing atmospheric Hg levels near the oldest chemical factory in central Europe using a tree ring archive
2022
Nováková, Tereza | Navratil, Tomas | Schütze, Martin | Rohovec, Jan | Matoušková, Šárka | Hošek, Michal | Matys Grygar, Tomáš
The Chemical Factory in Marktredwitz (CFM) is known as the oldest chemical factory in Germany (1778–1985), and from the beginning of the 20ᵗʰ century focused primarily on the production of mercury (Hg) compounds. Due to extensive pollution, together with employee health issues, the CFM was shut in 1985 by a government order and remediation works proceeded from 1986 to 1993. In this study, tree ring archives of European Larch (Larix decidua Mill.) were used to reconstruct changes of air Hg levels near the CFM. Mercury concentrations in larch boles decreased from 80.6 μg kg⁻¹ at a distance of 0.34 km–3.4 μg kg⁻¹ at a distance of 16 km. The temporal trend of atmospheric Hg emissions from the CFM reconstructed from the tree ring archives showed two main peaks. The first was in the 1920s, with a maximum tree ring Hg concentration 249.1 ± 43.9 μg kg⁻¹ coinciding with when the factory had a worldwide monopoly on the production of Hg-based seed dressing fungicide. The second peak in the 1970s, with a maximum tree ring Hg concentration of 116.4 ± 6.3 μg kg⁻¹, was associated with a peak in the general usage and production of Hg chemicals and goods. We used the tree ring record to reconstruct past atmospheric Hg levels using a simple model of Hg distribution between the larch tree rings and atmosphere. The precision of the tree ring model was checked against the results of air Hg measurements during the CFM remediation 30 years ago. According to the tree ring archives, the highest air Hg concentrations in the 1920s in Marktredwitz were over 70 ng m⁻³. Current air Hg levels of 1.18 ng m⁻³, assessed in the city of Marktredwitz, indicate the lowest air Hg in the past 150 years, underscoring the effective remediation of the CFM premises 30 years ago.
显示更多 [+] 显示较少 [-]Microwave-responsive SiC foam@zeolite core-shell structured catalyst for catalytic pyrolysis of plastics
2022
Chen, Zhaohui | Monzavi, Mohammad | Latifi, Mohammad | Samih, Said | Chaouki, J.
Catalytic pyrolysis is a promising chemical recycling technology to supplement mechanical recycling since plastics can be broken down into monomers or converted to the required fuels and chemicals. In this study, a microwave (MW) -responsive SiC foam@zeoltie core-shell structured catalyst was proposed for the catalytic pyrolysis of polyolefins. Under microwave irradiation, the SiC foam core works as both microwave adsorber and catalyst support, thus concentrating the generated heat energy on the ZSM-5 zeolite shell, where the catalytic reaction takes place. SiC foam with an open cellular structure can also improve the global transport of mass and heat during plastics pyrolysis. In this work, the effects of the SiO₂/Al₂O₃ ratio and alkaline treatment of ZSM-5 zeolite coated SiC foam under MW irradiation on the variations in product distribution from low-density polyethylene (LDPE) pyrolysis were investigated at 450 °C. The results indicated that the appropriate acidity and pore structure were crucial to upgrading gas and liquid products. Particularly, the creation of a mesoporous structure in ZSM-5 zeolite via alkaline treatment could improve the diffusion of large molecules and products, thus significantly increasing the selectivity of high-valued light olefins and aromatics while inhibiting the formation of unwanted alkanes, which are expected in the chemical industry. Concretely, the concentration of olefins in gas increased to 51.0 vol% for ZSM-5(50)-0.25AT, and 65.6 vol% for ZSM-5 (50)-0.50AT, compared with 45.2 vol% for the parent ZSM-5(50). The relative concentration of aromatics in liquid decreased from 96.6% for ZSM-5(50) to 75.9% for ZSM-5(50)-0.25AT, and 71.1% for ZSM-5(50)-0.50AT. Given the respective yield of gas and liquid, the total selectivity of C2–C4 olefins and aromatics for mesoporous ZSM-5 zeolites could reach 58.6–64.9% during LDPE pyrolysis, which were higher than that for the parent ZSM-5 zeolite.
显示更多 [+] 显示较少 [-]The occurrence, distribution and removal of adsorbable organic halogens (AOX) in a typical fine chemical industrial park
2022
Xu, Ranyun | Chi, Tongtong | Ren, Hang | Li, Feifei | Tian, Jinping | Chen, Lyujun
Coastal water quality in China has been impacted by direct discharge of industrial wastewater, and various kinds of AOX pollutants have been detected in the seawater and sediment. As the dominant pollution source of Hangzhou Bay, a typical fine chemical industry park “HSEDA” was selected as the study area in this research. The AOX in both wastewater and sludge phases from 22 large-scaled enterprises were simultaneously investigated. The results quantitatively illustrated the AOX flows from engineered wastewater and sludge treatment systems to natural environment. It can be seen that industrial enterprises discharged at least 160 t AOX every year, and about 105.4 t/a AOX eventually entered the natural environment. The dye manufacturing industry, which accounted for more than 60% of the total AOX emission load in HSEDA, was identified as the AOX pollution-intensive sector. The occurrence, characteristic pollutants and fate of AOX in dye wastewater were discussed, on the basis of which the improvements of cleaner production and wastewater treatment technologies have been put forward.
显示更多 [+] 显示较少 [-]Spatial distributions and sources of PAHs in soil in chemical industry parks in the Yangtze River Delta, China
2021
Jia, Tianqi | Guo, Wei | Xing, Ying | Lei, Rongrong | Wu, Xiaolin | Sun, Shurui | He, Yunchen | Liu, Wenbin
The Yangtze River Delta (YRD) is one of the fastest developing areas in eastern China and contains many chemical industry parks. The profiles and sources of polycyclic aromatic hydrocarbons (PAHs) in soil in chemical industry parks and surrounding areas in the YRD were investigated by analyzing soil samples (n = 64) were collected in the YRD and Rudong chemical park (RD), a typical chemical park in the Yangtze River Delta. The total concentrations of 19 PAHs in the YRD soil samples were 16.3–4694 ng g⁻¹ (mean 688 ng g⁻¹), and the total concentrations of PAHs in RD were 21.6–246 ng g⁻¹ (mean 75.4 ng g⁻¹). The PAHs in soil in YRD were dominated by four-ring and five-ring PAHs, and the PAHs in RD were dominated by two-ring and three-ring PAHs. It suggested that PAHs may have been supplied to soil in YRD predominantly through coal combustion and vehicle emissions, PAHs in the soil of RD may be due to the volatilization and leakage of chemical raw material. According to the different distribution characteristics of PAHs, the ratio (1.5) of (2 + 3) rings/4 rings was proposed to identify the chemical source of PAHs. The PAH isomer ratios and principal component analysis/multiple linear regression (PCA/MLRA) results indicated that PAHs concentrations in soil in the YRD and RD are mainly supplied by industrial and traffic emissions. Incremental lifetime cancer risks (ILCRs) indicated that PAHs in soil pose negligible cancer risks to children and adults, but much stronger risks to children than adults.
显示更多 [+] 显示较少 [-]Characteristics and health risks of benzene series and halocarbons near a typical chemical industrial park
2021
Chen, Ruonan | Li, Tingzhen | Huang, Chengtao | Yu, Yunjiang | Zhou, Li | Hu, Guocheng | Yang, Fumo | Zhang, Liuyi
Health risks of typical benzene series and halocarbons (BSHs) in a densely populated area near a large-scale chemical industrial park were investigated. Ambient and indoor air and tap water samples were collected in summer and winter; and the concentration characteristics, sources, and exposure risks of typical BSH species, including five benzene series (benzene, toluene, ethylbenzene, o-xylene, m,p-xylene) and five halocarbons (dichloromethane, trichloromethane, trichloroethylene, tetrachloromethane, and tetrachloroethylene), were analysed. The total mean concentrations of BSHs were 53.32 μg m⁻³, 36.29 μg m⁻³, and 26.88 μg L⁻¹ in indoor air, ambient air, and tap water, respectively. Halocarbons dominated the total BSHs with concentrations relatively higher than those in many other industrial areas. Industrial solvent use, industrial processes, and vehicle exhaust emissions were the principal sources of BSHs in ambient air. The use of household products (e.g., detergents and pesticides) was the principal source of indoor BSHs. Inhalation is the primary human exposure route. Ingestion of drinking water was also an important exposure route but had less impact than inhalation. Lifetime non-cancer risks of individual and cumulative BSHs were below the threshold (HQ = 1), indicating no significant lifetime non-cancer risks in the study area. However, tetrachloromethane, benzene, trichloromethane, ethylbenzene, and trichloroethylene showed potential lifetime cancer risk. The cumulative lifetime cancer risks exceeded the tolerable benchmark (1 × 10⁻⁴), indicating a lifetime cancer risk of BSHs to residents near the chemical industry park. This study provides valuable information for the management of public health in chemical industrial parks.
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