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Nanoporous bimetallic metal-organic framework (FeCo-BDC) as a novel catalyst for efficient removal of organic contaminants
2019
Li, Huanxuan | Zhang, Jian | Yao, Yuze | Miao, Xiangrui | Chen, Jiale | Tang, Junhong
In this work, we report on the synthesis and characterization of nanoporous bimetallic metal-organic frameworks (FeCo-BDC). Effects of synthesis time and temperature on the structures, morphology, and catalytic performance of FeCo-BDC were investigated. Scanning Electron Microscopy (SEM), Transmission electron microscopy (TEM) and Brunauer-Emmett-Teller (BET) were used to reveal the morphological and textural characteristics. The crystal structure and chemical composition of FeCo-BDC were determined by means of X-ray powder diffraction (XRD), Fourier Transform Infrared Spectroscopy (FT-IR), X-ray Photoelectron Spectroscopy (XPS), and Inductively Coupled Plasma Mass Spectrometry (ICP-MS) measurements. Interestingly, FeCo-BDC grew into the same crystal structure with different morphology in the temperature of 110–150 °C with 12–48 h. The heterogeneous catalytic activity of FeCo-BDC was tested to activate peroxydisulfate (PDS) and peroxymonosulfate (PMS) for removal of methylene blue (MB). The results found that FeCo-BDC synthesized at 150 °C with 24 h exhibited the best catalytic performance for PMS and obtained 100% of MB removal within 15 min. The abundant unsaturated metal active sites of Fe(II) and Co(II) in the skeleton of FeCo-BDC made a great contribution to the generation of sulfate (▪) and hydroxyl radicals (OH), which resulted in the excellent performance for MB degradation.
显示更多 [+] 显示较少 [-]Regulation of coastal methane sinks by a structured gradient of microbial methane oxidizers
2019
He, Zhanfei | Wang, Jiaqi | Hu, Jiajie | Yu, Hanqing | Jetten, Mike S.M. | Liu, Huan | Cai, Chaoyang | Liu, Yan | Ren, Hongxing | Zhang, Xu | Hua, Miaolian | Xu, Xinhua | Zheng, Ping | Hu, Baolan
Coastal wetlands are widely recognized as atmospheric methane sources. However, recent field studies suggest that some coastal wetlands could also act as methane sinks, but the mechanism is not yet clear. Here, we investigated methane oxidation with different electron acceptors (i.e., oxygen, nitrate/nitrite, sulfate, Fe(III) and Mn(IV)) in four coastal wetlands in China using a combination of molecular biology methods and isotopic tracing technologies. The geochemical profiles and in situ Gibbs free energies suggest that there was significant nitrite-dependent anaerobic oxidation of methane (nitrite-AOM) in the sub-surface sediments; this was subsequently experimentally verified by both the microbial abundance and activity. Remarkably, the methanotrophic communities seemed to exist in the sediments as layered structures, and the surface aerobic methane-oxidizing bacteria were able to take up atmospheric methane at a rate of 0.10–0.18 nmol CH₄ day⁻¹ cm⁻², while most, if not all, sedimentary methane was being completely consumed by anaerobic methanotrophs (23–58% by methane oxidizers in phylum NC10). These results suggest that coastal methane sinks might be governed by diverse microbial communities where NC10 methane oxidizers contributed significantly. This finding helps to better understand and predict the coastal methane cycle and reduce uncertainties in the estimations of the global methane flux.
显示更多 [+] 显示较少 [-]Response of Plantago major to cesium and strontium in hydroponics: Absorption and effects on morphology, physiology and photosynthesis
2019
Burger, Anna | Weidinger, Marieluise | Adlassnig, Wolfram | Puschenreiter, Markus | Lichtscheidl, Irene
Human activities lead to increasing concentration of the stable elements cesium (Cs) and strontium (Sr) and their radioactive isotopes in the food chain, where plants play an important part. Here we investigated Plantago major under the influence of long-term exposure to stable Cs and Sr.The plants were cultivated hydroponically in different concentrations of cesium sulfate (between 0.002 and 20 mM) and strontium nitrate (between 0.001 and 100 mM).Uptake of Cs and Sr into leaves was analyzed from extracts by inductively coupled plasma mass spectrometry (ICP-MS). It was increased with increasing external Cs and Sr concentrations. However, the efficiency of Cs and Sr transfer from solution to plants was higher for low external concentrations. Highest transfer factors were 6.78 for Cs and 71.13 for Sr. Accumulation of Sr was accompanied by a slight decrease of potassium (K) and calcium (Ca) in leaves, whereas the presence of Cs in the medium affected only uptake of K.The toxic effects of Cs and Sr were estimated from photosynthetic reactions and plant growth.In leaves, Cs and Sr affected the chlorophyll fluorescence even at their low concentrations. Low and high concentrations of both ions reduced dry weight and length of roots and leaves.The distribution of the elements between the different tissues of leaves and roots was investigated using Energy Dispersive X-Ray microanalysis (EDX) with scanning electron microscope (SEM). Overall, observations suggested differential patterns in accumulating Cs and Sr within the roots and leaves.When present in higher concentrations the amount of Cs and Sr transferred from environment to plants was sufficient to affect some physiological processes. The experimental model showed a potential for P. major to study the influence of radioactive contaminants and their removal from hotspots.
显示更多 [+] 显示较少 [-]Factors influencing methylmercury contamination of black bass from California reservoirs
2019
Melwani, Aroon R. | Negrey, John | Heim, Wes A. | Coale, Kenneth H. | Stephenson, Mark D. | Davis, Jay A.
Understanding how mercury (Hg) accumulates in the aquatic food web requires information on the factors driving methylmercury (MeHg) contamination. This paper employs data on MeHg in muscle tissue of three black bass species (Largemouth Bass, Spotted Bass, and Smallmouth Bass) sampled from 21 reservoirs in California. During a two-year period, reservoirs were sampled for total Hg in sediment, total Hg and MeHg in water, chlorophyll a, organic carbon, sulfate, dissolved oxygen, pH, conductivity, and temperature. These data, combined with land-use statistics and reservoir morphometry, were used to investigate relationships to size-normalized black bass MeHg concentrations. Significant correlations to black bass MeHg were observed for total Hg in sediment, total Hg and MeHg in surface water, and forested area. A multivariate statistical model predicted Largemouth Bass MeHg as a function of total Hg in sediment, MeHg in surface water, specific conductivity, total Hg in soils, and forested area. Comparison to historical reservoir sediment data suggested there has been no significant decline in sediment total Hg at five northern California reservoirs during the past 20 years. Overall, total Hg in sediment was indicated as the most influential factor associated with black bass MeHg contamination. The results of this study improve understanding of how MeHg varies in California reservoirs and the factors that correlate with fish MeHg contamination.
显示更多 [+] 显示较少 [-]Chemistry-triggered events of PM2.5 explosive growth during late autumn and winter in Shanghai, China
2019
Sun, Wenwen | Wang, Dongfang | Yao, Lan | Fu, Hongbo | Fu, Qingyan | Wang, Hongli | Li, Qing | Wang, Lin | Yang, Xin | Xian, Aiyong | Wang, Gehui | Xiao, Hang | Chen, Jianmin
To better understand the mechanism of PM₂.₅ explosive growth (EG), we conducted concurrent measurements of gaseous pollutants, PM₂.₅ and its chemical composition (inorganic ions, organic carbon, and element carbon) with a time resolution of 1 h in Shanghai in late autumn and winter from 2014 to 2017. In this study, the EG events, which are defined as the net increase in the mass concentration of PM₂.₅ by more than 100 μg m⁻³ within hours, are separately discussed for 3, 6, or 9 h. The number of EG events decreased from 19 cases in 2014 to 6 cases in 2017 and the corresponding PM₂.₅ concentration on average decreased from 183.6 μg m⁻³ to 128.8 μg m⁻³. Both regional transport and stagnant weather (windspeed < 2.0 m s⁻¹) could lead to EG events. The potential source contribution function (PSCF) shows that the major high-pollution region is in East China (including Zhejiang, Jiangsu, Shandong, and Anhui Province) and the North China Plain. The contribution of stagnant conditions to EG episode hours of 55% (198 h, 156.9 μg m⁻³) is higher than that of regional transport (45%, 230 h, 163.0 μg m⁻³). To study the impact of local emission, chemical characteristics and driving factors of EG were discussed under stagnant conditions. The major components contributing to PM₂.₅ are NO₃⁻ (17.9%), organics (14.1%), SO₄²⁻ (13.1%), and NH₄⁺ (13.1%). The driving factors of EG events are the secondary aerosol formation of sulfate and nitrate and primary emissions (vehicle emissions, fireworks, and biomass burning), but the secondary transformation contributes more to EG events. The formation of sulfate and nitrate is dominated by gas-phase oxidation and heterogeneous reactions, which are enhanced by a high relative humidity. The current study helps to understand the chemical mechanism of haze and provides a scientific basis for air pollution control in Shanghai.
显示更多 [+] 显示较少 [-]Biotoxicity of water-soluble species in PM2.5 using Chlorella
2019
Yang, Liu | Duan, Fengkui | Tian, Hua | He, Kebin | Ma, Yongliang | Ma, Tao | Li, Hui | Yang, Shuo | Zhu, Lidan
China has been faced with severe haze pollution, which is hazardous to human health. Among the air pollutants, PM2.5 (particles with an aerodynamic diameter ≤ 2.5 μm) is the most dangerous because of its toxicity and impact on human health and ecosystems. However, there has been limited research on PM2.5 particle toxicity. In the present study, we collected daily PM2.5 samples from January 1 to March 31, 2018 and selected samples to extract water-soluble species, including SO42−, NO3−, WSOC, and NH4+. These samples represented clean, good, slight, moderate, and heavy pollution days. After extraction using an ultrasonic method, PM2.5 solutions were obtained. We used Chlorella as the test algae and studied the content of chlorophyll a, as well as the variation in fluorescence when they were placed into the PM2.5 extraction solution, and their submicroscopic structure was analyzed using transmission electron microscopy (TEM). The results showed that when the air quality was relatively clean and good (PM2.5 concentration ≤ 75 μg m−3), the PM2.5 extraction solutions had no inhibiting effects on Chlorella, whereas when the air quality was polluted (PM2.5 concentration > 75 μg m−3) and heavily polluted (PM2.5 concentration > 150 μg m−3), with increasing PM2.5 concentrations and exposure time, the chlorophyll a content in Chlorella decreased. Moreover, the maximum photochemical quantum yield (Fv/Fm) of Chlorella obviously decreased, indicating chlorophyll inhibition during polluted days with increasing PM2.5 concentrations. The effects on the chlorophyll fluorescence parameters were also obvious, leading to an increase of energy dissipated per unit reaction center (DIo/RC), suggesting that Chlorella could survive when exposed to PM2.5 solutions, whereas the physiological activities were significantly inhibited. The TEM analysis showed that there were few effects on Chlorella cell microstructure during clean days, whereas plasmolysis occurred during light- and medium-polluted days. With increasing pollution levels, plasmolysis became more and more apparent, until the organelles inside the cells were thoroughly destroyed and most of the parts could not be recognized.
显示更多 [+] 显示较少 [-]Synergistic effects of anionic surfactants on adsorption of norfloxacin by magnetic biochar derived from furfural residue
2019
Li, Changjing | Gao, Yuan | Li, Aimin | Zhang, Lei | Ji, Guozhao | Zhu, Kongyun | Wang, Xuexue | Zhang, Yulin
Norfloxacin (NOR) is a persistent organic pollutant and can be effectively removed from effluent by adsorption of biochar. However, the presence of other emerging contaminants, such as surfactants, will potentially alter adsorption performance of norfloxacin by biochar and the molecular-scale mechanisms of the interaction between surfactants and biochar remain poorly understood. In this study, adsorption of norfloxacin on magnetic biochar prepared with iron-containing furfural residue (FRMB) in the presence or absence of anionic surfactants was investigated. The adsorption of NOR was significantly affected by the initial pH and anionic surfactants-sodium dodecyl sulfate (SDS) and sodium dodecyl benzene sulfonate (SDBS). In the presence of SDS and SDBS, the maximum sorption capacities of NOR were 2.33 and 1.97 times higher than that in the absence of surfactants, reached to 698.6 mg g⁻¹ and 589.9 mg g⁻¹, respectively. The optimal pH condition which was 4 indicated that electrostatic adsorption played a decisive role in the adsorption process after introduction of SDS/SDBS. The adsorption data were fitted well by the Elovich model and Freundlich model at the optimal conditions in which both SDS and SDBS were hemimicelle (0.8 mM SDS or 0.4 mM SDBS), indicating surface heterogeneity of FRMB and the adsorption mechanism was related to the assembly of surfactants on biochar. FTIR results showed that FRMB and SDS/SDBS interacted through hydrophobic action, and more complex or aggregates were formed between the NOR and biochar/SDS/SDBS. This work highlights the synergistic enhancement effects of tested surfactants on the removal of NOR by magnetic biochar from aqueous systems.
显示更多 [+] 显示较少 [-]Removal characteristics of a composite active medium for remediation of nitrogen-contaminated groundwater and metagenomic analysis of degrading bacteria
2019
Li, Shuo | Zhang, Yuling | Qian, Hong | Deng, Zhiqun | Wang, Xi | Yin, Siqi
To investigate the removal characteristics of ammonium-nitrogen (NH₄⁺-N), nitrite-nitrogen (NO₂⁻-N), nitrate-nitrogen (NO₃⁻-N), and total nitrogen from groundwater by a degradable composite active medium, kinetics, thermodynamics, and equilibrium adsorption, experiments were performed using scoria and degrading bacteria immobilized on scoria. Removal of NH₄⁺-N, NO₂⁻-N, and NO₃⁻-N was conducted in adsorption experiments using different times, initial concentrations, pH values, and groundwater chemical compositions (Ca²⁺, Mg²⁺, HCO₃⁻, CO₃²⁻, Fe²⁺, Mn²⁺, and SO₄²⁻). The results showed that the removal of nitrogen by the composite active medium was obviously better than that of scoria alone. The removal rates of NH₄⁺-N (C₀ = 5 mg/L), NO₂⁻-N (C₀ = 5 mg/L), and NO₃⁻-N (C₀ = 100 mg/L) by the composite active medium within 1 h were 96.05%, 82.40%, and 83.16%, respectively. The adsorption kinetics were well fitted to a pseudo-second order model, whereas the equilibrium adsorption agreed with the Freundlich model. With changes in the pH, variation in the removal could be attributed to the combined effect of hydrolysis and competitive ion adsorption, and the optimum pH was 7. Different concentration conditions, hardness, alkalinity, anions, and cations showed different promoting and inhibiting effects on the removal of nitrogen. A careful examination of ionic concentrations in adsorption batch experiments suggested that the sorption behavior of nitrogen onto the immobilized medium was mainly controlled by ion exchange. The degrading bacteria on the scoria surface were eluted and analyzed by metagenomic sequencing. There were significant differences in the number of operational taxons, relative abundances, and community diversity among degrading bacteria after adsorption of the three forms of nitrogen. The relative abundance of degrading bacteria was highest after NO₃⁻-N removal, and the diversity was highest after NO₂⁻-N removal. Pseudomonas and Serratia were the dominant genera that could efficiently remove NH₄⁺-N and NO₂⁻-N.
显示更多 [+] 显示较少 [-]Bacteriological and geochemical features of the groundwater resources: Kettara abandoned mine (Morocco)
2019
Zouhri, Lahcen | El Amari, Khalid | Marier, David | Benkaddour, Abdelfattah | Hibti, Mohamed
Waste water of the Kettara village, as well as the abandoned tailings, constitute a potential environmental issue with direct consequences on air, soil, water resources qualities and, on human health. In this paper, experimental investigations examine the environmental impact which is induced by the wastewater, mine tailings and the lithological factors of rocks. This multidisciplinary research allows to i) understand the transfer of the Metallic Trace Elements (selenium, arsenic, nickel and zinc) and sulfate ions in the fractured shales media, ii) to assess the water potability by using the microbiological analysis. The microbiological results reveal the domestic impact by the presence of several kinds of bacteria in the groundwater resources: E. coli, Fecal coliforms, Total coliforms, Enterococci, Mesophilic Aerobic Flora, Sulphite-reducing bacteria and Salmonella.Selenium, arsenic and the bacteriological contamination of the groundwater could be explained by five kinds of factors: i) the geological formations and the nature of the hydrogeological system (unconfined layer), ii) the groundwater flow, the hydraulic relation between the hydrogeological wells and, the fractures network in the shale aquifer. The piezometric map allows to highlight the groundwater flow from the North-East to North-West and to the South-West, the drainage axis towards the P21 well and the presence of the dividing axis in the contaminated zone by the arsenic, iii) the absence of the unhealthy habitats with permeable traditional septic tanks in the village; iv) the transfer of the spreading animal excrements from the soil to groundwater and, v) the migration of the wastewater towards downstream of the groundwater flow. The presence of the reed beds could explain the reduction of bacteria in the hydrogeological wells of the study area.
显示更多 [+] 显示较少 [-]Contributions of local pollution emissions to particle bioreactivity in downwind cities in China during Asian dust periods
2019
Ho, Kin-Fai | Wu, Kuan-Che | Niu, Xinyi | Wu, Yunfei | Zhu, Chong-Shu | Wu, Feng | Cao, Jun-Ji | Shen, Zhen-Xing | Hsiao, Ta-Chih | Chuang, Kai-Jen | Chuang, Hsiao-Chi
This study investigated the effects of pollution emissions on the bioreactivity of PM2.5 during Asian dust periods. PM2.5 during the sampling period were 104.2 and 85.7 μg m−3 in Xi'an and Beijing, respectively, whereas PM2.5 which originated from the Tengger Desert was collected (dust background). Pollution conditions were classified as non-dust days, pollution episode (PE), dust storm (DS)-1, and DS-2 periods. We observed a significant decrease in cell viability and an increase in LDH that occurred in A549 cells after exposure to PM2.5 during a PE and DS-1 in Xi'an and Beijing compared to Tengger Desert PM2.5. Positive matrix factorization was used to identify pollution emission sources. PM2.5 from biomass and industrial sources contributed to alterations in cell viability and LDH in Xi'an, whereas vehicle emissions contributed to LDH in Beijing. OC, EC, Cl−, K+, Mg2+, Ca, Ti, Mn, Fe, Zn, and Pb were correlated with cell viability and LDH for industrial emissions in Xi'an during DS. OC, EC, SO42−, S, Ti, Mn, and Fe were correlated with LDH for vehicle emissions in Beijing during DS. In conclusion, the dust may carry pollutants on its surface to downwind areas, leading to increased risks of particle toxicity.
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