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Distribution of florfenicol and norfloxacin in ice during water freezing process: Dual effects by fluorine substituents
2022
Sun, Heyang | Chen, Tianyi | Zhang, Liwen | Dong, Deming | Li, Yanchun | Guo, Zhiyong
Distribution in ice is regarded as one of important transport modes for pollutants in seasonal freeze-up waters in cold regions. However, the distribution characteristics and mechanisms of fluorinated antibiotics as emerging contaminants during the water freezing process remain unclear. Here, florfenicol and norfloxacin were selected as model fluorinated antibiotics to investigate their ice-water distribution. Effects of antibiotic molecular structure on the distribution were explored through comparative studies with their non-fluorinated structural analogs. Results showed that phase changes during the ice growth process redistributed the antibiotics, with antibiotic concentrations in water 3.0–6.4 times higher than those in ice. The solute-rich boundary layer with a concentration gradient was presented at the ice-water interface and controlled by constitutional supercooling during the freezing process. The ice-water distribution coefficient (KIW) values of antibiotics increased by 34.8%–38.0% with a doubling of the cooling area. The solute distribution coefficient (Kbₛ) values of antibiotics at −20 °C were 65.6%–70.3% higher than at −10 °C. The KIW and Kbₛ values of all antibiotics were negatively correlated with their water solubilities. The fluorine substituents influenced the binding energies between antibiotics and ice, resulting in a 1.1-fold increase in the binding energy of norfloxacin on the ice surface relative to its structural analog pipemidic acid. The results provide a new insight into the transport behaviors of fluorinated pharmaceuticals in ice-water systems.
Показать больше [+] Меньше [-]Accumulation characteristic of nitrogen in reservoirs during the ice-covered period under superimposed influence of ice and sediments: A case study of Biliuhe reservoir
2022
Hu, Suduan | Wang, Tianxiang | Xu, Shiguo | Ma, Lingxiao | Wang, Tianzi | Sun, Ya
Reservoirs located in middle and high latitudes freeze for months in winter, where the accumulation characteristics of pollutants are changed by superimposed influence of salt exclusion from ice on the surface and pollution release from sediments at the bottom. Taking total nitrogen (TN) of Biliuhe reservoir in Northeast China as an example, we developed a model to simulate TN accumulation characteristics influenced by ice and sediments during the freezing period (NACISF), and quantified contributions of TN from ice and sediments. Model parameters of ice and sediments were determined by laboratory freeze-up simulation experiment and sediment release flux simulation experiment, and water quality data were obtained from field investigations. Results showed that the annual average amount of TN input during the ice-covered period from 2015 to 2020 was 220.77 t, the output was 400.11 t, and the accumulated amount was 589.52 t. TN excluded from ice and released from sediments contributed 8.12% and 7.17% of the total TN inputs in winter, respectively. Analysis showed that the TN excluded from ice was positively correlated with ice thickness and initial TN concentration. The maximum ice thickness of Biliuhe reservoir had a 13 year cyclic feature, and the proportion of TN excluded from ice to the total TN inputs in different periods ranged from 10.68% to 17.30% (mean 13.18%). Meanwhile, TN accumulated seasonally as summer > autumn > winter > spring. The TN exclusion effect in 2050 would be weakened when considering the combined effects of climate change and human activities, with a reduction of about 40.85% compared to the current. It is concluded that the NACISF model took into account the influences of both ice and sediments, which provided a detailed understanding of the accumulation characteristics of TN during freezing period, and had important reference significance for water quality management in winter.
Показать больше [+] Меньше [-]Effect of fulvic acid concentration levels on the cleavage of piperazinyl and defluorination of ciprofloxacin photodegradation in ice
2022
Li, Zhuojuan | Dong, Deming | Zhang, Liwen | Li, Yanchun | Guo, Zhiyong
Ice is an important physical and chemical sink for various pollutants in cold regions. The photodegradation of emerging fluoroquinolone (FQ) antibiotic contaminants with dissolved organic matter (DOM) in ice remains poorly understood. Here, the photodegradation of ciprofloxacin (CIP) and fulvic acid (FA) in different proportions as representative FQ and DOM in ice were investigated. Results suggested that the photodegradation rate constant of CIP in ice was 1.9 times higher than that in water. When CFA/CCIP ≤ 60, promotion was caused by FA sensitization. FA increased the formation rate of cleavage in the piperazine ring and defluorination products. When 60 < CFA/CCIP < 650, the effect of FA on CIP changed from promoting to inhibiting. When 650 ≤ CFA/CCIP ≤ 2600, inhibition was caused by both quenching effects of 143.9%–51.3% and light screening effects of 0%–48.7%. FA inhibited cleavage in the piperazine ring for CIP by the scavenging reaction intermediate of aniline radical cation in ice. When CFA/CCIP > 2600, the light screening effect was greater than the quenching effect. This work provides new insights into how DOM affects the FQ photodegradation with different concentration proportions, which is beneficial for understanding the environmental behaviors of fluorinated pharmaceuticals in cold regions.
Показать больше [+] Меньше [-]Continuously observed light absorbing impurities in snow cover over the southern Altai Mts. in China: Concentrations, impacts and potential sources
2021
Zhong, Xinyue | Kang, Shichang | Zhang, Wei | Yang, Junhua | Niu, Hewen | Liu, Yajun | Guo, Junming | Li, Xiaofei | Chen, Pengfei | Wang, Xiaoxiang
The deposition of light absorbing impurities (LAIs) (e.g., black carbon (BC), organic carbon (OC), mineral dust (MD)) on snow is an important attribution to accelerate snowmelt across the northern Xinjiang, China. At present, there is still a lack of understanding of the LAIs concentration, elution and enrichment process in snow cover over Xinjiang. Based on these, continuously sampling during two years carried out to investigate the concentrations, impacts and potential sources of LAIs in snow at Kuwei Station in the southern Altai Mountains. The average concentrations of BC, OC and MD in the surface snow were 2787 ± 2334 ng g⁻¹, 6130 ± 6127 ng g⁻¹, and 70.03 ± 62.59 μg g⁻¹, respectively, which dramatically increased along with snowmelt intensified, reflecting a significant enrichment process of LAIs at the snow surface. Besides, high LAIs concentrations also found in the subsurface and melting layers of the snowpit, reflecting the elution and redistribution of LAIs. With the simulation of the SNow ICe Aerosol Radiative model, BC was the main dominant factor in reducing snow albedo and radiative forcing (RF), its impact was more remarkable in the snowmelt period. The average contribution rates of BC, MD and BC + MD to snow albedo reduction increased by 20.0 ± 1.9%, 13.0 ± 0.2%, and 20.5 ± 2.3% in spring compared with that in winter; meanwhile, the corresponding average RFs increased by 15.8 ± 3.4 W m⁻², 4.7 ± 0.3 W m⁻² and 16.4 ± 3.2 W m⁻², respectively. Changes in the number of snowmelt days caused by BC and MD decreased by 3.0 ± 0.4 d to 8.3 ± 1.3 d. It indicated that surface enrichment of LAIs during snow melting might accelerate snowmelt further. Weather Research and Forecasting Chemistry model showed that the resident emission was the main potential source of BC and OC in snow. This implied that the mitigation of intensive snowmelt needs to mainly reduce resident emission of LAIs in the future.
Показать больше [+] Меньше [-]Elevated cadmium pollution since 1890s recorded by forest chronosequence in deglaciated region of Gongga, China
2020
Wang, Xun | Luo, Ji | Lin, Che-Jen | Wang, Dingyong | Yuan, Wei
Ice and sediment cores, peat bogs and tree rings are useful proxy records for reconstructing historical air pollution events. However, these indirect measurements are subject to interferences caused by environmental perturbations including global climate change. Therefore, using multiple proxy records has advantages in constraining the analytical findings. In this study, we utilized the chronological record of atmospheric deposition preserved in vegetation succession ecosystems in the deglaciated region for reconstructing historical pollution events. The rate of Cd accumulation in the forest chronosequence zone was investigated in a deglaciated area of the Tibetan Plateau. The results obtained through this novel approach are consistent with the variations of Cd concentration recorded in tree-ring, showing a 4–7 times increase of atmospheric Cd deposition from the 1890s to the early 1970s followed by a decrease from the mid-1970s–2000s. The Cd pollution record indicates that elevated atmospheric Cd release occurred in regions of Southwest China and South Asia due to the rapid industrial development until 1970 followed by coordinated efforts in controlling air emissions after mid-1970s.
Показать больше [+] Меньше [-]Iced block method: An efficient method for preparation of micro-sized expanded polystyrene foams
2020
Kwak, Jin Il | An, Youn-Joo
Recently, numerous studies concerning dye-labeled microplastic beads have reported on the end-of-life, environmental effects of microplastics because of their ubiquitous commercial usage. Less is understood about the toxicity and bioaccumulation of plastics other than microplastic beads, which can also harm the environment (e.g., fragments, fibers, foams, and films). Expanded polystyrene (EPS) is widespread in the environment owing to its many uses, however, limited research has been conducted on EPS foams. This study focuses on developing an efficient method for the preparation of micro-sized EPS foams for research purposes and compares it with previous microplastics preparation methods reported in 68 previous studies. It was demonstrated that the iced EPS block method (iced EPS block + water) generated larger quantities of smaller-sized EPS foams (20–200 and 200–500 μm) compared to the EPS + ice + water and EPS + water methods. The optimal protocol includes 1) iced EPS block preparation, 2) grinding and sieving, and 3) collecting. Additionally, it was confirmed that the iced EPS block method requires less money, labor, and time compared to previously reported methods in the literature. The method proposed in this research can assist future investigations into the environmental effects of EPS foams.
Показать больше [+] Меньше [-]Aromatic acids as biomass-burning tracers in atmospheric aerosols and ice cores: A review
2019
Wan, Xin | Kawamura, Kimitaka | Ram, Kirpa | Kang, Shichang | Loewen, Mark | Gao, Shaopeng | Wu, Guangming | Fu, Pingqing | Zhang, Yanlin | Bhattarai, Hemraj | Cong, Zhiyuan
Biomass burning (BB) is one of the largest sources of carbonaceous aerosols with adverse impacts on air quality, visibility, health and climate. BB emits a few specific aromatic acids (p-hydroxybenzoic, vanillic, syringic and dehydroabietic acids) which have been widely used as key indicators for source identification of BB-derived carbonaceous aerosols in various environmental matrices. In addition, measurement of p-hydroxybenzoic and vanillic acids in snow and ice cores have revealed the historical records of the fire emissions. Despite their uniqueness and importance as tracers, our current understanding of analytical methods, concentrations, diagnostic ratios and degradation processes are rather limited and scattered in literature. In this review paper, firstly we have summarized the most established methods and protocols for the measurement of these aromatic acids in aerosols and ice cores. Secondly, we have highlighted the geographical variability in the abundances of these acids, their diagnostic ratios and degradation processes in the environments. The review of the existing data indicates that the concentrations of aromatic acids in aerosols vary greatly with locations worldwide, typically more abundant in urban atmosphere where biomass fuels are commonly used for residential heating and/or cooking purposes. In contrast, their concentrations are lowest in the polar regions which are avoid of localized emissions and largely influenced by long-range transport. The diagnostic ratios among aromatic acids can be used as good indicators for the relative amounts and types of biomass (e.g. hardwood, softwood and herbaceous plants) as well as photochemical oxidation processes. Although studies suggest that the degradation processes of the aromatic acids may be controlled by light, pH and hygroscopicity, a more careful investigation, including closed chamber studies, is highly appreciated.
Показать больше [+] Меньше [-]Experimental determination of drift and PM10 cooling tower emissions: Influence of components and operating conditions
2017
Ruiz, J. | Kaiser, A.S. | Lucas, M.
Cooling tower emissions have become an increasingly common hazard to the environment (air polluting, ice formation and salts deposition) and to the health (Legionella disease) in the last decades. Several environmental policies have emerged in recent years limiting cooling tower emissions but they have not prevented an increasing intensity of outbreaks.Since the level of emissions depends mainly on cooling tower component design and the operating conditions, this paper deals with an experimental investigation of the amount of emissions, drift and PM10, emitted by a cooling tower with different configurations (drift eliminators and distribution systems) and working under several operating conditions. This objective is met by the measurement of cooling tower source emission parameters by means of the sensitive paper technique. Secondary objectives were to contextualize the observed emission rates according to international regulations.Our measurements showed that the drift rates included in the relevant international standards are significantly higher than the obtained results (an average of 100 times higher) and hence, the environmental problems may occur. Therefore, a revision of the standards is recommended with the aim of reducing the environmental and human health impact. By changing the operating conditions and the distribution system, emissions can be reduced by 52.03% and 82% on average. In the case of drift eliminators, the difference ranges from 18.18% to 98.43% on average. As the emissions level is clearly influenced by operating conditions and components, regulation tests should be referred to default conditions. Finally, guidelines to perform emission tests and a selection criterion of components and conditions for the tested cooling tower are proposed.
Показать больше [+] Меньше [-]Levoglucosan evidence for biomass burning records over Tibetan glaciers
2016
You, Chao | Xu, Chao | Xu, Baiqing | Zhao, Huabiao | Song, Lili
Intense biomass burning (BB) events are widespread in tropical and subtropical Asia. However, the impact of BB aerosols on the Tibetan Plateau (TP), especially on Tibetan glaciers, is poorly understood. In this study, BB signals are revealed using the specific molecular tracer levoglucosan in snow and ice samples from different Tibetan glaciers. Tibetan glaciers mainly act as receptors of BB emissions from surrounding regions. Significant differences in levoglucosan concentrations in glacier samples collected from two slopes on the same mountain range indicate that high mountains can act as natural barriers to block the transport of smoke aerosols to the TP. Levoglucosan concentrations show a decreasing trend from west to east on glaciers impacted by the Indian summer monsoon on the southern edge of the TP, while the opposite pattern was observed on glaciers under the prevailing westerlies along the northern edge. The emission sources, the controlling climate system, as well as deposition and degradation during transport determined the spatial distribution regimes of levoglucosan concentration on Tibetan glaciers.
Показать больше [+] Меньше [-]Global-scale patterns in anthropogenic Pb contamination reconstructed from natural archives
2016
Marx, Samuel K. | Rashid, Shaqer | Stromsoe, Nicola
During the past two centuries metal loads in the Earth's atmosphere and ecosystems have increased significantly over pre-industrial levels. This has been associated with deleterious effects to ecosystem processes and human health. The magnitude of this toxic metal burden, as well as the spatial and temporal patterns of metal enrichment, is recorded in sedimentary archives across the globe. This paper presents a compilation of selected Pb contamination records from lakes (n = 10), peat mires (n = 10) and ice fields (n = 7) from Europe, North and South America, Asia, Australia and the Northern and Southern Hemisphere polar regions. These records quantify changes in Pb enrichment in remote from source environments. The presence of anthropogenic Pb in the environment has a long history, extending as far back as the early to mid-Holocene in North America, Europe and East Asia. However, results show that Pb contamination in the Earth's environment became globally ubiquitous at the beginning of the Second Industrial Revolution (c.1850–1890 CE), after which the magnitude of Pb contamination increased significantly. This date therefore serves as an effective global marker for the onset of the Anthropocene. Current global average Pb enrichment rates are between 6 and 35 times background, however Pb contamination loads are spatially variable. For example, they are >100 times background in Europe and North America and 5–15 times background in Antarctica. Despite a recent decline in Pb loads in some regions, most notably Europe and North America, anthropogenic Pb remains highly enriched and universally present in global ecosystems, while concentrations are increasing in some regions (Australia, Asia and parts of South America and Antarctica). There is, however, a paucity of Pb enrichment records outside of Europe, which limits assessments of global contamination.
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