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Characterization of dicarboxylic acids, oxoacids, and α-dicarbonyls in PM2.5 within the urban boundary layer in southern China: Sources and formation pathways Full text
2021
Liu, Jianing | Zhou, Shengzhen | Zhang, Zhimin | Kawamura, Kimitaka | Zhao, Wanyu | Wang, Xuemei | Shao, Min | Jiang, Fan | Liu, Junwen | Sun, Xi | Hang, Jian | Zhao, Jun | Pei, Chenglei | Zhang, Jingpu | Fu, Pingqing
Low-molecular-weight dicarboxylic acids, which are important components of secondary organic aerosols, have been extensively studied in recent years. Many studies have focused on ground-level observations and literature reports on the vertical distribution of the organic aerosols within the urban boundary layer are limited. In this study, the vertical profiles of dicarboxylic acids and related organic compounds (DCRCs) in PM₂.₅ were investigated at altitudinal levels (ground level and 488 m above the ground level) at the Canton Tower in Guangzhou, southern China, to elucidate their primary sources and secondary formation processes. The concentrations of DCRCs at ground level were generally higher than those at 488 m. Oxalic acid (C₂) was the most abundant species, followed by succinic acid (C₄) and malonic acid (C₃) at both heights. The higher ratio of DCRCs-bound carbon to organic carbon (i.e., DCRCs-C/OC) at 488 m (4.8 ± 1.2%) relative to that at ground level (2.7 ± 0.5%) indicated a higher degree of aerosol aging at 488 m. The abundance of C₂ was increased and the conversion of C₄ to C₃ was enhanced due to the photochemical oxidation of its homologues during long-range transport periods. The increase in C₂ was associated with in-cloud processes during pollution periods. Principal component analysis showed that DCRCs were mainly derived from atmospheric secondary processing and biomass burning was also an important source of long-chain carboxylic acids during autumn in Guangzhou. Our results illustrate that secondary processing and biomass burning play prominent roles in controlling the abundance of DCRCs. Furthermore, DCRCs are affected by air masses from regional areas, oxidation of their precursors via vertical transport and in-cloud processes.
Show more [+] Less [-]Yeast biomass-induced Co2P/biochar composite for sulfonamide antibiotics degradation through peroxymonosulfate activation Full text
2021
Peng, Yuanyuan | Tong, Wenhua | Xie, Yi | Hu, Wanrong | Li, Yonghong | Zhang, Yongkui | Wang, Yabo
Advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) activation have attracted increasing attention in recent years for organic pollutants removal. Herein, we put forward a facile method to form cobalt phosphide/carbon composite for PMS activation. Combining impregnation approach with pyrolysis treatment enabled the formation of Co₂P/biochar composites using baker’s yeast and Co²⁺ as precursors. The as-synthesized products exhibited excellent catalytic activity for sulfamethoxazole (SMX) degradation over the pH range 3.0–9.0 b y activating PMS. For example, 100% of SMX (20 mg L⁻¹) removal was achieved in 20 min with catalyst dosage of 0.4 g L⁻¹ and PMS loading of 0.4 g L⁻¹. Near zero Co²⁺ leaching was observed during catalytic reaction, which remarkably lowered the toxic risk of transition metal ion in water. Meanwhile, the reusability of catalyst could be attained by thermal treatment. SMX degradation intermediates were identified by liquid chromatography-mass spectrometry (LC-MS), which facilitated the proposal of possible SMX degradation pathways. Ecological Structure Activity Relationships (ECOSAR) analysis indicated that SMX degradation intermediates may not pose ecological toxicity to the environment. Further investigation verified that Co₂P/biochar composites could set off PMS activation not only for the degradation of SMX but also for other sulfonamides. In this study, we not only developed a facile method of utilizing environmental-benign biomass for transition metal phosphide/carbon composite formation, but also achieved highly efficient antibiotic elimination by PMS-based AOP.
Show more [+] Less [-]Mapping high resolution national daily NO2 exposure across mainland China using an ensemble algorithm Full text
2021
Liu, Jianjun
Nitrogen dioxide (NO₂) is an important air pollutant and highly related to air quality, short- and long-term health effects, and even climate. A national model was developed using the extreme gradient boosting algorithm with high-resolution tropospheric vertical column NO₂ densities from the Sentinel-5 Precursor/Tropospheric Monitoring Instrument and general meteorological variables as input to generate daily mean surface NO₂ concentrations across mainland China. Model-derived daily NO₂ estimates were high accuracy with sample-based cross-validation coefficient of determination of 0.83, a root-mean-square error of 7.58 μg/m³, a mean prediction error of 5.56 μg/m³, and a mean relative prediction error of 18.08%. It has good performance in NO₂ estimations at both regional and individual site scale. The model also performed well in terms of estimating monthly, seasonal, and annual mean NO₂ concentrations across China. The model performance appears to better than or comparable to most previous related studies. The seasonal and annual spatial distributions of surface NO₂ across China and several regional NO₂ hotspots in 2019 were derived from the model and analyzed. Also evaluated were the population exposure levels of NO₂ for cities in and provinces of China. At the national scale, about 12% of the population experienced annual mean NO₂ concentrations exceeding the Chinese national air quality standard. The nationwide model with conventional predictors developed here can derive high-resolution surface NO₂ concentrations across China routinely, benefitting air epidemiological and environmental related studies.
Show more [+] Less [-]Energy and environmental applications of Sn4+/Ti4+ doped α-Fe2O3@Cu2O/CuO photoanode under optimized photoelectrochemical conditions Full text
2021
Nagappagari, Lakshmana Reddy | Lee, Jaewon | Lee, Hyeonkwon | Jeong, Beomgyun | Lee, Kiyoung
The most promising technique for directly converting solar energy into clean fuels and environmental remediation by organic dye degradation is photoelectrochemical (PEC) process. We introduced Sn⁴⁺/Ti⁴⁺ doped α-Fe₂O₃@CuₓO heterojunction photoanode with complete optimization for PEC hydrogen (H₂) generation and organic dye degradation. Improvement of photocurrent photo and reducing overpotentials under optimized conditions lead to enhancing PEC performances, degradation efficiency of organic compounds, and H₂ generation generation rate. The optimized heterojunction photoanode (5TiFe@CuₓO-D) showed IPCE exceeding 42% compared with pristine hematite (Fe₀.₀₁–800₆ₕ) nanostructures (28%). Additionally, all the optimized photoanodes showed higher PEC stability for 10 h. Time-resolved PL spectra confirm the improved average lifetime for heterojunction photoanodes, supporting the enhanced PEC performance. Optimized 5TiFe@CuₓO-D material achieved PEC H₂ generation of ∼300 μL h⁻¹.cm⁻² which is two times higher than pristine hematite’s activity (150 μL h⁻¹.cm⁻²) and almost 99% degradation efficiency within 120 min of irradiation time. Therefore, a state-of-the-art study has been explored for hematite-based heterojunction photoanodes reflecting the superior PEC performance and hydrogen, methyl orange (MO) dye degradation activities. The improved results were reported because of stable morphology and better crystallinity acquired through systematic investigation of thermal effects and hydrothermal duration, improved electrical properties by Sn/Ti doping into the lattice of α-Fe₂O₃ and optimization of CuₓO deposition methods. The formation of well-defined heterojunction minimizes the recombination of the charge carrier and leads to effective transportation of excited electrons for the enhanced PEC performance.
Show more [+] Less [-]Ecotoxicological effects of pyraclostrobin on tilapia (Oreochromis niloticus) via various exposure routes Full text
2021
Li, Hong | Jing, Tongfang | Li, Tongbin | Huang, Xueping | Gao, Yangyang | Zhu, Jiamei | Lin, Jin | Zhang, Peng | Li, Beixing | Mu, Wei
Pyraclostrobin is a widely used and highly efficient fungicide that also has high toxicity to aquatic organisms, especially fish. Although some research has reported the toxic effects of pyraclostrobin on fish, the main toxic pathways of pyraclostrobin in fish remain unclear. The present study has integrated histopathological, biochemical and hematological techniques to reveal the main toxic pathways and mechanisms of pyraclostrobin under different exposure routes. Our results indicated that pyraclostrobin entered fish mainly through the gills. The highest accumulation of pyraclostrobin was observed in the gills and heart compared with accumulation in other tissues and gill tissue showed the most severe damage. Hypoxia symptoms (water jacking, tummy turning and cartwheel formation) in fish were observed throughout the experiment. Taken together, our results suggested that the gills are important target organs. The high pyraclostrobin toxicity to gills might be associated with oxidative damage to the gills, inducing alterations in ventilation frequency, oxygen-carrying substances in blood and disorders of energy metabolism. Our research facilitates a better understanding of the toxic mechanisms of pyraclostrobin in fish, which can promote the ecotoxicological research of agrochemicals on aquatic organisms.
Show more [+] Less [-]Removal of urban-use insecticides in a large-scale constructed wetland Full text
2021
Cryder, Zachary | Wolf, Douglas | Carlan, Craig | Gan, Jay
Water treatment and reuse initiatives are essential to combat declining water supplies in a changing climate, especially in arid and semi-arid regions. Pollution of water resources intensifies the search for strategies to provide water for potable and non-potable reuse that mitigates detrimental ecological and human health effects. Fipronil and synthetic pyrethroids are common urban-use insecticides that exert aquatic toxicity at trace levels and have been often found in urban surface streams. In this study, samples were collected from the 182 ha Prado Wetlands in Southern California for seven months to assess the occurrence of fipronil and its degradation products as well as pyrethroids (bifenthrin and cyfluthrin) in water, sediment, and plants in a 4.45 ha vegetated surface flow constructed wetland (CW). Concentration-based removal values and changes in mass flux were calculated to determine the efficacy of CW treatment. Observed water concentrations were further used to calculate toxic units for the invertebrates Hyalella azteca and Chironomus dilutus. Pesticide concentrations in water, sediment, and plant samples consistently decreased during passage through the CW at all time points. Removal values for fipronil desulfinyl, fipronil sulfide, fipronil, fipronil sulfone, bifenthrin, and cyfluthrin were 100%, 99.7–100%, 57.8–88.1%, 75.6–100%, 74.7–100%, and 36.6–82.2%, respectively, and there was a general net deposition of pesticides into CW compartments. Toxic unit values decreased in every instance for both aquatic invertebrates. Settling of contaminated particles, adsorption to sediment, plant uptake or adsorption, and subsequent degradation contributed to the effective removal of these urban-use insecticides, which highlights the potential of CWs for protecting urban water quality.
Show more [+] Less [-]Associations of urinary carbon disulfide metabolite with oxidative stress, plasma glucose and risk of diabetes among urban adults in China Full text
2021
Xu, Tao | Wang, Bin | Wang, Xing | Yang, Shijie | Cao, Limin | Qiu, Weihong | Cheng, Man | Liu, Wei | Yu, Linling | Zhou, Min | Wang, Dongming | Ma, Jixuan | Chen, Weihong
Carbon disulfide (CS₂) has been reported to induce disorder of glucose metabolism. However, the associations of CS₂ exposure with plasma glucose levels and risk of diabetes have not been explored in general population, and the underlying mechanisms remain unclear. We aim to examine the relationships between CS₂ exposure and fasting plasma glucose (FPG) levels, as well as diabetes, and assess the potential role of oxidative stress among the abovementioned relationships in Chinese general adults. The concentrations of urinary biomarkers of CS₂ exposure (2-thiothiazolidin-4-carboxylic acid, TTCA), and biomarkers for lipid peroxidation (8-isoprostane, 8-iso-PGF₂α) and DNA oxidative damage (8-oxo-7,8-dihydro-20-deoxyguanosine, 8-OHdG) were measured among 3338 urban adults from the Wuhan-Zhuhai cohort. Additionally, FPG levels were tested promptly. Generalized linear models and logistic regression models were used to quantify the associations among urinary TTCA, oxidative damage markers, FPG levels and diabetes risk. Mediation analysis was employed to estimate the role of oxidative damage markers in the association between urinary TTCA and FPG levels. We discovered a significant relationship between urinary TTCA and FPG levels with regression coefficient of 0.080 (95% CI: 0.002,0.157). Besides, the risk of diabetes was positively related to urinary TTCA (OR:1.282, 95% CI: 1.055,1.558), particularly among those who did not exercise regularly. Each 1% increase of urinary TTCA concentration was associated with a 0.096% and 0.037% increase in urinary 8-iso-PGF₂α and 8-OHdG, respectively. Moreover, we found an upward trend of FPG level as urinary 8-iso-PGF₂α gradually increased (Pₜᵣₑₙd<0.05), and urinary 8-iso-PGF₂α mediated 21.12% of the urinary TTCA-associated FPG increment. Our findings indicated that urinary CS₂ metabolite was associated with increased FPG levels and diabetes risk in general population. Lipid peroxidation partly mediated the association of urinary CS₂ metabolite with FPG levels.
Show more [+] Less [-]Human health risks estimations from polycyclic aromatic hydrocarbons in serum and their hydroxylated metabolites in paired urine samples Full text
2021
Yang, Ziying | Guo, Chongshan | Li, Qin | Zhong, Yi | Ma, Shengtao | Zhou, Jinhua | Li, Xiaotong | Huang, Rende | Yu, Yingxin
Polycyclic aromatic hydrocarbons (PAHs) are compounds with two or more benzene rings whose hydroxylated metabolites (OH-PAHs) are excreted in urine. Human PAH exposure is therefore commonly estimated based on urinary OH-PAH concentrations. However, no study has compared PAH exposure estimates based on urinary OH-PAHs to measurements of PAH levels in blood samples. Estimates of PAH exposure based solely on urinary OH-PAHs may thus be subject to substantial error. To test this hypothesis, paired measurements of parent PAHs in serum and OH-PAHs in urine samples from 480 participants in Guangzhou, a typical developed city in southern China, were used to investigate differences in the estimates of human PAH exposure obtained by sampling different biological matrices. The median PAH concentration in serum was 4.05 ng mL⁻¹, which was lower than that of OH-PAHs in urine (8.33 ng mL⁻¹). However, serum pyrene levels were significantly higher than urinary levels of its metabolite 1-hydroxypyrene. Concentrations of parent PAHs in serum were not significantly correlated with those of their metabolites in urine with the exception of phenanthrene, which exhibited a significant negative correlation. Over 28% of the participants had carcinogenic risk values above the acceptable cancer risk level of 10⁻⁶. Overall, estimated human exposure and health risks based on urinary 1-hydroxypyrene levels were only 13.6% of those based on serum pyrene measurements, indicating that estimates based solely on urine sampling may substantially understate health risks due to PAH exposure.
Show more [+] Less [-]Environmental behavior and safety of polyhalogenated carbazoles (PHCZs): A review Full text
2021
Ji, Chenyang | Chen, Da | Zhao, Meirong
Polyhalogenated carbazoles (PHCZs) are well-known as emergent environmental contaminants. Given their wide distribution in the environment and structural similarity with dioxins and dioxin-like chemicals (DLCs), the environmental behavior and ecological risks of these chemicals have become the major issue concerned by the governments and scientists. Since the initial report of PHCZ residues in the environment in the 1980s, over 20 PHCZ congeners with different residual levels had been identified in various environmental media all over the world. Nevertheless, researches concerning the toxicological effects of PHCZs are of an urgent need for the relatively lagging study of their ecological risks. Currently, only limited evidence has indicated that PHCZs would pose dioxin-like toxicity, including developmental toxicity, cardiotoxicity, etc; and their toxicological effects were partially consistent with AhR activation. And yet, much remains to be done to fill in the knowledge gaps of their toxicological effects. In this review, the research progresses in environmental behavior and toxicology study of PHCZs were remarked; and the lack of current research, as well as future research prospects, were discussed.
Show more [+] Less [-]Nitrogen of EDDS enhanced removal of potentially toxic elements and attenuated their oxidative stress in a phytoextraction process Full text
2021
Beiyuan, Jingzi | Fang, Linchuan | Chen, Hansong | Li, Mengdi | Liu, Dongdong | Wang, Yunqiang
(S,S)-ethylenediaminedisuccinic acid (EDDS) has a strong capacity to mobilize potentially toxic elements (PTEs) in phytoextraction. It can release NH₄⁺-N via biodegradation, which can enhance N supply to soil thereafter promote plant growth and plant resistance to PTEs. However, the advanced feature of released N in the EDDS-enhanced phytoextraction remains unclear. In the current study, the effects of N supply released from EDDS on ryegrass phytoextraction and plant resistance to PTEs were investigated in detail by a comparison with urea. Our results supported that the addition of both EDDS and urea increased N concentration in soil solution, yet EDDS needed more time to release available N for plant uptake and transported more N from root to shoot. Additionally, EDDS significantly increased the concentration of all targeted PTEs, i.e. Cu, Zn, Cd, and Pb, in the soil solution, which results in higher levels of their occurrence in plant biomass compared with urea. By contrast, the supply of N slightly enhanced the ryegrass uptake of micro-nutrients, i.e. Cu and Zn, yet it caused negligible effects on nonessential elements, i.e. Cd and Pb. The mobilized PTEs by EDDS lead to elevated oxidative stress because higher levels of malondialdehyde and O₂•⁻ were observed. The supply of N attenuated oxidative stress caused by O₂•⁻ and H₂O₂, which was associated with enhanced activities of superoxide dismutase and peroxidase. Our results advanced the understanding of the exogenous N supply and metal resistance mechanisms in the EDDS-enhanced phytoextraction. This study also highlighted that EDDS can serve as a N source to ease N-deficient problems in PTEs-contaminated soils.
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