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Photolytic kinetics of pharmaceutically active compounds from upper to lower estuarine waters: Roles of triplet-excited dissolved organic matter and halogen radicals Full text
2021
Hou, Zhichao | Fang, Qi | Liu, Huaying | Li, Yingjie | Zhao, Qun | Zhang, Zhiyu | Lei, Yajie | Tian, Senlin
Photodegradation is a major elimination route of many pharmaceutically active compounds (PhACs) in natural surface waters, yet their photolytic behavior in estuarine waters with salinity gradient change is largely unknown. Herein, sulfamethazine and carbamazepine were taken as representative PhACs to explore the photolytic kinetic differences in Qinzhou Bay estuarine water samples collected from upper to lower reaches. Rapid photodegradation of sulfamethazine was found in lower estuarine water relative to upstream estuarine water; whereas for carbamazepine, photolytic rate was inversely proportional to the salinity of estuarine waters. Experiments with extracted estuarine dissolved organic matter (E-DOM) imply that the multivariate effects of triplet-excited E-DOM (³E-DOM∗) and halide ions are responsible for the enhancement photolysis of sulfamethazine. Radical scavenging experiments suggest that the photolysis enhancement can be ascribed to the contribution of reactive halogen species (RHS), while their contribution to carbamazepine is negligible and ³E-DOM∗ is the dominant reactive species for its photodegradation. This indicates that the reactivity differences with RHS and ³DOM∗ affect the photolytic kinetics of PhACs from upper estuarine waters to lower reaches, which is also supported by a good linear relationship between the ratios of photolytic rates for ten PhACs in E-DOM solution with/without halides and the ratios of the reactivity of these pollutants with RHS and ³DOM∗. These findings show that the different reactivity of PhACs with ³E-DOM∗ and RHS influences the photolytic kinetics in estuarine waters with different salinity, and highlights the photochemical behavior of organic micropollutants from upstream to downstream estuarine waters.
Show more [+] Less [-]Advances in Ultra-Trace Analytical Capability for Micro/Nanoplastics and Water-Soluble Polymers in the Environment: Fresh Falling Urban Snow Full text
2021
Wang, Zi | Saadé, Nadim K. | Ariya, Parisa A.
Discarded micro/nano-plastic inputs into the environment are emerging global concerns. Yet the quantification of micro/nanoplastics in complex environmental matrices is still a major challenge, notably for soluble ones. We herein develop in-laboratory built nanostructures (zinc oxide, titanium oxide and cobalt) coupled to mass spectrometry techniques, for picogram quantification of micro/nanoplastics in water and snow matrices, without sample pre-treatment. In parallel, an ultra-trace quantification method for micro/nanoplastics based on nanostructured laser desorption/ionization time-of-flight mass spectrometry (NALDI-TOF-MS) is developed. The detection limit is ∼5 pg for ambient snow. Soluble polyethylene glycol and insoluble polyethylene fragments were observed and quantified in fresh falling snow in Montreal, Canada. Complementary physicochemical studies of the snow matrices and reference plastics using laser-based particle sizers, inductively coupled plasma tandem mass spectrometry, and high-resolution scanning/transmission electron microscopy, produced consistent results with NALDI, and further provided information on morphology and composition of the micro/nano-plastic particles. This work is promising as it demonstrates that a wide range of recyclable nanostructures, in-laboratory built or commercial, can provide ultra-trace capability for quantification for both soluble polymers and insoluble plastics in air, water and soil. It may thereby produce key missing information to determine the fate of micro/nanoplastics in the environment, and their impacts on human health.
Show more [+] Less [-]Mitigation potential of black carbon emissions from on-road vehicles in China Full text
2021
Zhang, Shaojun | Wu, Xiaomeng | Zheng, Xuan | Wen, Yifan | Wu, Ye
Black carbon (BC) is the most potent light-absorbing component of particulate matter and can have a significant warming impact. On-road vehicles are a major source of BC and a significant contributor to global warming. This paper establishes an updated inventory to quantify the mitigation potential of efforts to control BC emissions from on-road transportation in China. The total emissions of BC from on-road vehicles in China were 152.1 thousand tons in 2017. Heavy-duty diesel fleets accounted for a large percentage of emissions, whereas light-duty gasoline fleets presented a gradually increasing trend of emissions. Historically, comprehensive control policies for on-road vehicle emissions have achieved substantial BC reductions, with a 45% decrease in 2017 compared to 2000. With the implementation of stringent control policies and the development of advanced control technologies, BC emissions from the on-road sector may have a greater reduction potential in the future. By 2035, three various future scenarios representing different stringency levels of emission controls will reduce BC emissions by 58%, 90%, and 93% relative to 2017. The major benefits in reducing BC emissions result from more stringent emission standards and the accelerated retirement of older heavy-duty diesel vehicles. The shorter lifetime of BC than that of CO₂ implies that the mitigation of BC emissions would offer an important opportunity to contribute to alleviating global warming in the short term. Our assessment reveals that in 2035, the most stringent scenario, Scenario PC3, could deliver a CO₂-equivalent emission reduction on a 20-year scale of 234.2 (GWP₂₀₋yᵣ) million tons compared with the NAP Scenario, which is equivalent to reducing the oil consumption in China’s transportation sector by nearly 20% from a climate impact perspective.
Show more [+] Less [-]Prenatal exposure to bisphenol analogues and digit ratio in children at ages 4 and 6 years: A birth cohort study Full text
2021
Wang, Ziliang | Zhou, Yan | Liang, Hong | Miao, Maohua | Chen, Yafei | Zhang, Xiaotian | Song, Xiuxia | Yuan, Wei
Bisphenol analogues (BPs), including bisphenol A (BPA), have been shown to exhibit similar endocrine disrupting activities. However, epidemiological evidence on the reproductive and developmental toxicities of BPs other than BPA is scarce. The second to fourth digit ratio (2D:4D), an endocrine-sensitive endpoint, has been suggested to be a biomarker of prenatal sex steroid exposure and associated with reproductive outcomes in later life. Using the data of 545 mother-child pairs from the Shanghai-Minhang Birth Cohort Study, we prospectively assessed the effects of prenatal exposure to BPs on 2D:4D in children at ages 4 and 6 years. Single-spot urine samples were collected in the third trimester and analyzed for BPs. Digit lengths were measured using a vernier caliper in children at ages 4 and 6 years, and the 2D:4D values for both hands were calculated. A multivariable linear regression model was applied to examine associations between prenatal BPs exposure and 2D:4D digit ratios at each age separately. The generalized estimating equation (GEE) model was used to deal with repeated 2D:4D measures obtained at ages 4 and 6 years. We found that prenatal exposure to BPA alternatives including BPF, BPS, and BPAF was associated with higher digit ratio in boys and/or girls (feminizing), while TCBPA, a halogenated bisphenol, was associated with lower 2D:4D in boys (masculinizing). These associations were more pronounced at 4 years of age, and tended to remain after further considering the potential confounding from prenatal co-exposure to other BPs and childhood BPs exposure. Our study provides epidemiological evidence that BPs exposure during pregnancy may alter the digit development in children, indicative of disrupted reproductive development in later life. Given these new findings, further studies are needed to corroborate our results.
Show more [+] Less [-]Responses of juvenile fathead minnow (Pimephales promelas) gut microbiome to a chronic dietary exposure of benzo[a]pyrene Full text
2021
DeBofsky, Abigail | Xie, Yuwei | Challis, Jonathan K. | Jain, Niteesh | Brinkmann, Markus | Jones, Paul D. | Giesy, John P.
The microbiome has been described as an additional host “organ” with well-established beneficial roles. However, the effects of exposures to chemicals on both structure and function of the gut microbiome of fishes are understudied. To determine effects of benzo[a]pyrene (BaP), a model persistent organic pollutant, on structural shifts of gut microbiome in juvenile fathead minnows (Pimephales promelas), fish were exposed ad libitum in the diet to concentrations of 1, 10, 100, or 1000 μg BaP g⁻¹ food, in addition to a vehicle control, for two weeks. To determine the link between exposure to BaP and changes in the microbial community, concentrations of metabolites of BaP were measured in fish bile and 16S rRNA amplicon sequencing was used to evaluate the microbiome. Exposure to BaP only reduced alpha-diversity at the greatest exposure concentrations. However, it did alter community composition assessed as differential abundance of taxa and reduced network complexity of the microbial community in all exposure groups. Results presented here illustrate that environmentally-relevant concentrations of BaP can alter the diversity of the gut microbiome and community network connectivity.
Show more [+] Less [-]Cascading effects of insecticides and road salt on wetland communities Full text
2021
Lewis, Jacquelyn L. | Agostini, Gabriela | Jones, Devin K. | Relyea, Rick A.
Novel stressors introduced by human activities increasingly threaten freshwater ecosystems. The annual application of more than 2.3 billion kg of pesticide active ingredient and 22 billion kg of road salt has led to the contamination of temperate waterways. While pesticides and road salt are known to cause direct and indirect effects in aquatic communities, their possible interactive effects remain widely unknown. Using outdoor mesocosms, we created wetland communities consisting of zooplankton, phytoplankton, periphyton, and leopard frog (Rana pipiens) tadpoles. We evaluated the toxic effects of six broad-spectrum insecticides from three families (neonicotinoids: thiamethoxam, imidacloprid; organophosphates: chlorpyrifos, malathion; pyrethroids: cypermethrin, permethrin), as well as the potentially interactive effects of four of these insecticides with three concentrations of road salt (NaCl; 44, 160, 1600 Cl⁻ mg/L). Organophosphate exposure decreased zooplankton abundance, elevated phytoplankton biomass, and reduced tadpole mass whereas exposure to neonicotinoids and pyrethroids decreased zooplankton abundance but had no significant effect on phytoplankton abundance or tadpole mass. While organophosphates decreased zooplankton abundance at all salt concentrations, effects on phytoplankton abundance and tadpole mass were dependent upon salt concentration. In contrast, while pyrethroids had no effects in the absence of salt, they decreased zooplankton and phytoplankton density under increased salt concentrations. Our results highlight the importance of multiple-stressor research under natural conditions. As human activities continue to imperil freshwater systems, it is vital to move beyond single-stressor experiments that exclude potentially interactive effects of chemical contaminants.
Show more [+] Less [-]Microbial mechanisms related to the effects of bamboo charcoal and bamboo vinegar on the degradation of organic matter and methane emissions during composting Full text
2021
Guo, Honghong | Gu, Jie | Wang, Xiaojuan | Song, Zilin | Yu, Jing | Lei, Liusheng
In this study, functional microbial sequencing, quantitative PCR, and phylogenetic investigation of communities by reconstruction of unobserved states (PICRUSt) were employed to understand the microbial mechanisms related to the effects of bamboo charcoal (BC) and bamboo vinegar (BV) on the degradation of organic matter (OM) and methane (CH₄) emissions during composting. BC + BV resulted in the highest degradation of OM. BV was most effective treatment in controlling CH₄ emissions and it significantly reduced the abundance of the mcrA gene. Methanobrevibacter, Methanosarcina, and Methanocorpusculum were closely related to CH₄ emissions during the thermophilic composting period. PICRUSt analysis showed that BC and/or BV enhanced the metabolism associated with OM degradation and reduced CH₄ metabolism. Structural equation modeling indicated that BC + BV strongly promoted the metabolic activity of microorganisms, which had a positive effect on CH₄ emissions. Together these results suggest that BC + BV may be a suitable composting strategy if the aerobic conditions can be effectively improved during the thermophilic composting period.
Show more [+] Less [-]Multigenerational selection towards longevity changes the protective role of vitamin C against graphene oxide-induced oxidative stress in house crickets Full text
2021
Flasz, Barbara | Dziewięcka, Marta | Kędziorski, Andrzej | Tarnawska, Monika | Augustyniak, Jan | Augustyniak, Maria
This research was designed to investigate changes that can arise in an invertebrate organism due to stress caused by a strong prooxidant, graphene oxide (GO), and a potent antioxidant, vitamin C. The study aimed to investigate if vitamin C may support convalescence after chronic GO intoxication. We investigated the toxicity of chronic dietary graphene oxide administration in house cricket (Acheta domesticus) types: wild and selected for longevity (with a better developed antioxidant system, conducive to long life). Vitamin C was applied immediately after cessation of graphene oxide intoxication to check if it can support the remedial effect. The condition of cells, DNA stability, catalase activity, and the reproduction potential, measured as the Vitellogenin (Vg) protein expression level, were investigated in control and GO treated groups, recovery groups (-GO), and recovery groups with Vit. C (-GO + Vit.C). In this study vitamin C had no evident remedial effect on the house crickets exposed to graphene oxide. Most probably, the mechanism of vitamin C action, in case of intoxication with nanoparticles, is much more complicated. In the context of the results obtained, it is worth considering whether Vit. C, applied after GO intoxication, causes further disturbance of homeostasis in terms of the cells' redox potential.
Show more [+] Less [-]Assessing the potential to use CDOM as an indicator of water quality for the sediment-laden Yellow river, China Full text
2021
Li, Dianbao | Pan, Baozhu | Han, Xu | Li, Junhua | Zhu, Qingwei | Li, Ming
Chromophoric dissolved organic matter (CDOM) in rivers is mainly affected by natural conditions and human activities and can reflect the watershed pollution status to a certain extent. The Yellow River is one of the largest contributors to the global riverine sediment flux from the land to ocean, and there is a paucity of information on how the optical properties of CDOM have the potential to serve as an indicator of water quality for the sediment-laden Yellow River. In this study, a three-dimensional fluorescence parallel factor (PARAFAC) analysis method was applied to investigate the seasonal and spatial variations in CDOM fluorescence components and spectral characteristics from the source region to the estuary in the mainstream of Yellow River. The relationships of CDOM with water quality indicators and trophic state were also analyzed. Six PARAFAC components (C1–C6) were identified and grouped into two categories: humic-like components (C1–C4), which accounted for 85.8 %, and protein-like components (C5 and C6), which accounted for only 14.2 %. The CDOM components, spectral parameters, and their clear correlations with the main ions (Na⁺ and Cl⁻) all indicated that the humic-like components may be primarily derived from nonpoint source erosion, and the protein-like components were mainly derived from point source discharges in the watershed. The combination of the CDOM absorption coefficient at 254 nm (a(254)), spectral slope ratio (SR), specific UV absorbance SUVA₂₅₄, and fluorescence index (FI) had a good predictive ability for the key water quality indicators (total nitrogen (TN), dissolved total nitrogen (DTN), total phosphorus (TP), dissolved total phosphorus (DTP), and chlorophyll a (Chl a)) and trophic state index (TSI). Therefore, some fluorophores and UV spectral parameters of CDOM in the Yellow River can be used for rapid water quality monitoring and pollution source indication, especially pollutants related to nitrogen and phosphorus nutrients in the basin.
Show more [+] Less [-]Fluorescent and colorimetric dual-mode detection of tetracycline in wastewater based on heteroatoms-doped reduced state carbon dots Full text
2021
Fu, Qing | Long, Caicheng | Qin, Lingfeng | Jiang, Zixin | Qing, Taiping | Zhang, Peng | Feng, Bo
A large amount of tetracycline (TC) persists in water, soil, food, and feed due to the overuse of antibiotics, causing serious environmental problems such as damage to ecosystems and posing risks to human health. Thus, there is an urgent need to find a method to detect TC that is practical, rapid, sensitive, and offers ready visualization of TC levels so that adequate remediation measures can be immediately implemented. Herein, we report a fluorescent and colorimetric dual-mode nanosensor for the detection of TC based on reduced state carbon dots (r-CDs). In the presence of TC, the emission fluorescence of r-CDs was quenched by the Förster resonance energy transfer mechanism to achieve high-sensitivity detection of TC with a low limit of detection (LOD) of 1.73 nM. Moreover, TC was also detected by r-CDs via a noticeable color change of the solution (from colorless to red) with the naked eye, having an LOD of 0.46 μM. Furthermore, r-CDs have excellent selectivity and sensitivity in detecting TC in wastewater, and therefore, have practical applications in wastewater treatment. The fluorescent and colorimetric dual-mode proposed in this work may offer a unique idea for the detection of TC, with great prospects for environmental wastewater applications.
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