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Polycyclic Aromatic Hydrocarbons (PAHs) in inland aquatic ecosystems: Perils and remedies through biosensors and bioremediation
2018
Behera, Bijay Kumar | Das, Abhishek | Sarkar, Dhruba Jyoti | Weerathunge, Pabudi | Parida, Pranaya Kumar | Das, Basantakumar | Thavamani, Palanisami | Ramanathan, Rajesh | Bansal, Vipul
Polycyclic Aromatic Hydrocarbons (PAHs) are among the most ubiquitous environmental pollutants of high global concern. PAHs belong to a diverse family of hydrocarbons with over one hundred compounds known, each containing at least two aromatic rings in their structure. Due to hydrophobic nature, PAHs tend to accumulate in the aquatic sediments, leading to bioaccumulation and elevated concentrations over time. In addition to their well-manifested mutagenic and carcinogenic effects in humans, they pose severe detrimental effects to aquatic life. The high eco-toxicity of PAHs has attracted a number of reviews, each dealing specifically with individual aspects of this global pollutant. However, efficient management of PAHs warrants a holistic approach that combines a thorough understanding of their physico-chemical properties, modes of environmental distribution and bioaccumulation, efficient detection, and bioremediation strategies. Currently, there is a lack of a comprehensive study that amalgamates all these aspects together. The current review, for the first time, overcomes this constraint, through providing a high level comprehensive understanding of the complexities faced during PAH management, while also recommending future directions through potentially viable solutions. Importantly, effective management of PAHs strongly relies upon reliable detection tools, which are currently non-existent, or at the very best inefficient, and therefore have a strong prospect of future development. Notably, the currently available biosensor technologies for PAH monitoring have not so far been compiled together, and therefore a significant focus of this article is on biosensor technologies that are critical for timely detection and efficient management of PAHs. This review is focussed on inland aquatic ecosystems with an emphasis on fish biodiversity, as fish remains a major source of food and livelihood for a large proportion of the global population. This thought provoking study is likely to instigate new collaborative approaches for protecting aquatic biodiversity from PAHs-induced eco-toxicity.
Показать больше [+] Меньше [-]Correlations and adsorption mechanisms of aromatic compounds on biochars produced from various biomass at 700 °C
2018
Yang, Kun | Jiang, Yuan | Yang, Jingjing | Lin, Daohui
Knowledge of adsorption behavior of organic contaminants on high heat temperature treated biochars is essential for application of biochars as adsorbents in wastewater treatment and soil remediation. In this study, isotherms of 25 aromatic compounds adsorption on biochars pyrolyzed at 700 °C from biomass including wood chips, rice straw, bamboo chips, cellulose, lignin and chitin were investigated to establish correlations between adsorption behavior and physicochemical properties of biochars. Isotherms were well fitted by Polanyi theory-based Dubinin-Ashtakhov (DA) model with three parameters, i.e., adsorption capacity (Q⁰) and adsorption affinity (E and b). Besides the negative correlation of Q⁰ with molecular maximum cross-sectional areas (σ) of organic compounds, positive correlations of Q⁰ with total pore volume (Vₜₒₜₐₗ) and average diameter of micropore (D) of biochars were observed, indicating that adsorption by biochars is captured by the pore-filling mechanism with molecular sieving effect in biochar pores. Linear solvation energy relationships (LSERs) of adsorption affinity (E) with solvatochromic parameters of organic compounds (i. e., αₘ and π∗) were established, suggesting that hydrophobic effect, π-π interaction and hydrogen-bonding interaction are the main forces responsible for adsorption. The regression coefficient (π₁) and intercept (C) of obtained LSERs are correlated with biochar H/C and Rₘᵢcᵣₒ, respectively, implying that biochars with higher aromaticity and more micropores have stronger π-π bonding potential and hydrophobic effect potential with aromatic molecule, respectively. However, hydrogen-bonding potential of biochars for organic molecules is not changed significantly with properties of biochars. A negative correlation of b with biochar H/C is also obtained. These correlations could be used to predict the adsorption behavior of organic compounds on high heat temperature treated biochars from various biomass for the application of biochars as sorbents and for the estimating of environmental risks of organic compounds in the present of biochars.
Показать больше [+] Меньше [-]Source apportionment for fine particulate matter in a Chinese city using an improved gas-constrained method and comparison with multiple receptor models
2018
Shi, Guoliang | Liu, Jiayuan | Wang, Haiting | Tian, Yingze | Wen, Jie | Shi, Xurong | Feng, Yinchang | Ivey, Cesunica E. | Russell, Armistead G.
PM₂.₅ is one of the most studied atmospheric pollutants due to its adverse impacts on human health and welfare and the environment. An improved model (the chemical mass balance gas constraint-Iteration: CMBGC-Iteration) is proposed and applied to identify source categories and estimate source contributions of PM₂.₅. The CMBGC-Iteration model uses the ratio of gases to PM as constraints and considers the uncertainties of source profiles and receptor datasets, which is crucial information for source apportionment. To apply this model, samples of PM₂.₅ were collected at Tianjin, a megacity in northern China. The ambient PM₂.₅ dataset, source information, and gas-to-particle ratios (such as SO₂/PM₂.₅, CO/PM₂.₅, and NOx/PM₂.₅ ratios) were introduced into the CMBGC-Iteration to identify the potential sources and their contributions. Six source categories were identified by this model and the order based on their contributions to PM₂.₅ was as follows: secondary sources (30%), crustal dust (25%), vehicle exhaust (16%), coal combustion (13%), SOC (7.6%), and cement dust (0.40%). In addition, the same dataset was also calculated by other receptor models (CMB, CMB-Iteration, CMB-GC, PMF, WALSPMF, and NCAPCA), and the results obtained were compared. Ensemble-average source impacts were calculated based on the seven source apportionment results: contributions of secondary sources (28%), crustal dust (20%), coal combustion (18%), vehicle exhaust (17%), SOC (11%), and cement dust (1.3%). The similar results of CMBGC-Iteration and ensemble method indicated that CMBGC-Iteration can produce relatively appropriate results.
Показать больше [+] Меньше [-]Destruction processes of mining on water environment in the mining area combining isotopic and hydrochemical tracer
2018
Yang, Yonggang | Guo, Tingting | Jiao, Wentao
There is less research on the hydrological system and its destruction processes mechanism in the mining areas, especially combined application of isotope technology and chemical signals, which is a key scientific problem that need to be solved. This study takes Jinci spring area in Shanxi as a case study. It is based on the data of hydrology and mining condition from 1954 to 2015, combining monitoring experiments, O18, D, S34 and N15 tracing, chemical and model simulation. This study investigates the hydrological regularity and impacts of mining activities on water quantity and quality, and reveals the destruction process of hydrological system. The results show that: (1) Water chemical type shows an evolutionary trend of HCO3−-Ca2+-Mg2+→SO42--HCO3--Ca2+-Mg2+→SO42--Ca2+-Mg2+, due to the influence of exploitation and fault zones. Isotope tracer shows that mine pit water is formed by a mixture of pore water, karst water and surface water. (2) Although precipitation and seepage have a certain impact on the reducing of groundwater quantity, over-exploitation of water resource is still the main reason for reducing of groundwater quantity. Under the conditions of keeping the exploitation intensity at the current level or reducing it by 10%, groundwater level shows a declining trend. Under the condition of reducing it by 30%, groundwater level starts to rise up. When reducing by 50%, groundwater level reaches its highest point. Coalmining changes the runoff, recharge and discharge paths. (3) From 1985 to 2015, Water quality in the mining area is worsening. Ca2+ increases by 35.30%, SO42− increases by 52.80%, and TDS (Total Dissolved Solid) increases by 67.50%. Nitrates come from the industrial and domestic wastewater, which is generated by mining. The percentage of groundwater coming from gypsum dissolusion is 67.51%, and the percentage from coal measure strata water is 34.49%. The water qualities of river branches are generally deteriorated.
Показать больше [+] Меньше [-]Associations of multiple plasma metals with incident type 2 diabetes in Chinese adults: The Dongfeng-Tongji Cohort
2018
Yuan, Yu | Xiao, Yang | Yu, Yanqiu | Liu, Yiyi | Feng, Wei | Qiu, Gaokun | Wang, Hao | Liu, Bing | Wang, Jing | Zhou, Lue | Liu, Kang | Xu, Xuedan | Yang, Handong | Li, Xiulou | Qi, Lu | Zhang, Xiaomin | He, Meian | Hu, Frank B. | Pan, An | Wu, Tangchun
The long-term associations between multiple metals and incident diabetes are uncertain. We aimed to examine the relationship between plasma concentrations of 23 metals and the incidence of type 2 diabetes among Chinese senior adults. We quantified fasting plasma concentrations of 23 metals by inductively coupled plasma mass spectrometry among 1039 incident diabetes cases and 1039 controls (age and sex matched) nested in a prospective study, the Dongfeng-Tongji cohort. Both cases and controls were free of diabetes at baseline (2008–2010), incident diabetes were identified using the following criteria: fasting glucose ≥ 7.0 mmoL/l; or hemoglobin A1c (HbA1c) ≥ 6.5%; or self-reported physician diagnosis of diabetes or use of anti-diabetic medication during the follow-up visits in 2013. In the conditional logistic regression models, the multivariable adjusted ORs (95% CIs) of diabetes across quartiles (Q1–Q4) of metal concentrations were as follows: titanium, 1.00, 0.92, 1.31, 1.38 (1.00–1.91, Ptrend = 0.011); selenium, 1.00, 1.08, 1.45, 1.27 (0.93–1.74, Ptrend = 0.05); and antimony, 1.00, 0.79, 0.77, 0.60 (0.44–0.83, Ptrend = 0.002). Arsenic was significantly associated with diabetes in the crude model (ORs comparing extreme quartiles 1.30; 1.02–1.65; Ptrend = 0.006), but was not significant after adjustment for socio-demographic factors. No significant associations were found for other metals. In conclusion, titanium and selenium were positively while antimony was negatively associated with incident diabetes.
Показать больше [+] Меньше [-]Mechanism of matrix-bound phosphine production in response to atmospheric elevated CO2 in paddy soils
2018
An, Shaorong | Niu, Xiaojun | Chen, Weiyi | Sheng, Hong | Lai, Senchao | Yang, Zhiquan | Gu, Xiaohong | Zhou, Shaoqi
To explore the effect of elevated CO₂ concentrations ([CO₂]) on phosphine formation in paddy fields, the matrix-bound phosphine (MBP) content, different phosphorus fractions and various carbon forms in soil samples from rice cultivation under varying CO₂ concentrations of 400 ppm, 550 ppm and 700 ppm by indoor simulation experiment were determined. This study showed that MBP concentration did not increase significantly with elevated [CO₂] over four-week cultivation periods of rice seedlings, regardless of soil layers. MBP had a significant positive correlation with total phosphorus (TP) and inorganic phosphorus (IP), and multiple stepwise linear regression analysis further indicated that MBP preservation in neutral paddy soils with depths of 0–20 cm may have been due to conversion from FeP and CaP. Based on redundancy analysis and forward selection analysis, speculated that the formation of MBP in the neutral paddy soils as the response to atmospheric elevated [CO₂] was due to two processes: (i) FeP transformation affected by the changes of soil respiration (SCO₂) and TOC was the main precursor for the production of MBP; and (ii) CaP transformation resulting from variation in HCO₃⁻ was the secondary MBP source. The complex combination of these two processes is simultaneously controlled by SCO₂. In a word, the soil environment in the condition of elevated [CO₂] was in favor of MBP storage in neutral paddy soils. The results of our study imply that atmospheric CO₂ participates in and has a certain impact on the global biogeochemical cycle of phosphorus.
Показать больше [+] Меньше [-]Ultrafine particle emissions from modern Gasoline and Diesel vehicles: An electron microscopic perspective
2018
Liati, Anthi | Schreiber, Daniel | Arroyo Rojas Dasilva, Yadira | Dimopoulos Eggenschwiler, Panayotis
Ultrafine (<100 nm) particles related to traffic are of high environmental and human health concern, as they are supposed to be more toxic than larger particles. In the present study transmission electron microscopy (TEM) is applied to obtain a concrete picture on the nature, morphology and chemical composition of non-volatile ultrafine particles in the exhaust of state-of-the-art, Euro 6b, Gasoline and Diesel vehicles. The particles were collected directly on TEM grids, at the tailpipe, downstream of the after-treatment system, during the entire duration of typical driving cycles on the chassis dynamometer. Based on TEM imaging coupled with Energy Dispersive X-ray (EDX) analysis, numerous ultrafine particles could be identified, imaged and analyzed chemically. Particles <10 nm were rarely detected. The ultrafine particles can be distinguished into the following types: soot, ash-bearing soot and ash. Ash consists of Ca, P, Mg, Zn, Fe, S, and minor Sn compounds. Most elements originate from lubricating oil additives; Sn and at least part of Fe are products of engine wear; minor W ± Si-bearing nearly spherical particles in Diesel exhaust derive from catalytic coating material. Ultrafine ash particles predominate over ultrafine soot or are nearly equal in amount, in contrast to emissions of larger sizes where soot is by far the prevalent particle type. This is probably due to the low ash amount per volume fraction in the total emissions, which does not favor formation of large ash agglomerates, opposite to soot, which is abundant and thus easily forms agglomerates of sizes larger than those of the ultrafine range. No significant differences of ultrafine particle characteristics were identified among the tested Gasoline and Diesel vehicles and driving cycles. The present TEM study gives information also on the imaging and chemical composition of the solid fraction of the unregulated sub-23 nm size category particles.
Показать больше [+] Меньше [-]Photodegradation of 17β-estradiol on silica gel and natural soil by UV treatment
2018
Wang, Siyuan | Wang, Xinghao | Li, Chenguang | Xu, Xinxin | Wei, Zhongbo | Wang, Zunyao | Qu, Ruijuan
This paper evaluates the UV photodegradation of 17β-estradiol (E2) on silica gel and in natural soil with different soil components. Silica gel was chosen as a stable and pure support to simulate the photochemical behavior of E2 on the surface of natural soil. Ultraviolet light, rather than visible light, was confirmed to play a decisive role in the photodegradation of E2 on silica gel. The effect of three soil components, including humic acid (HA), inorganic salts, and relative humidity (RH), on the photochemical behavior of E2 on silica gel or soil under UV irradiation was then evaluated. Two HA concentrations (10 and 20 mg g⁻¹) and three salts (ferric sulfate, copper sulfate and sodium carbonate) were observed to obviously inhibit the degradation of E2 on silica gel. Interestingly, nitrate was found to obviously improve the removal efficiency of E2. Both too-dry and too-wet conditions obviously reduced the removal rate of E2, and the optimum relative humidity (RH) value was found to be approximately about 35% (30 °C). Furthermore, twenty intermediate products and two major pathways were proposed to describe the transformation processes of E2 treated by UV irradiation, among which oligomers were found to be the major intermediate products before complete mineralization. The efficient UV removal of E2 on silica gel and natural soil suggested a feasible strategy to remediate E2 contaminated soil.
Показать больше [+] Меньше [-]Rapid debromination of polybrominated diphenyl ethers (PBDEs) by zero valent metal and bimetals: Mechanisms and pathways assisted by density function theory calculation
2018
Wang, Rui | Tang, Ting | Lu, Guining | Huang, Kaibo | Yin, Hua | Lin, Zhang | Wu, Fengchang | Dang, Zhi
Polybrominated diphenyl ethers (PBDEs) undergo debromination when they were exposed in zerovalent metal or bimetallic systems. Yet their debromination pathways and mechanisms in these systems were not well understood. Here we reported the debromination pathways of three BDE congeners (BDE-21, 25 and 29) by nano-zerovalent iron (n-ZVI). All these BDE congeners have three bromine substituents that were located in ortho-, meta- and para-positions. Results demonstrated that BDE-21, 25 and 29 preferentially debrominate meta-, ortho- and para-bromines, respectively, suggesting that bromine substituent at each position (i.e. ortho-, meta- or para-) of PBDEs can be preferentially removed. Singly occupied molecular orbitals of BDE anions are well correlated with their actual debromination pathways, which successfully explain why these BDE congeners exhibit certain debromination pathways in n-ZVI system. In addition, microscale zerovalent zinc (m-ZVZ), iron-based bimetals (Fe/Ag and Fe/Pd) were also used to debrominate PBDEs, with BDE-21 as target pollutant. We found that the debromination pathways of BDE-21 in m-ZVZ and Fe/Ag systems are the same to those in n-ZVI system, but were partially different from those in Fe/Pd systems. The debromination of BDE-21 in Pd-H2 system as well as the solvent kinetic isotope effect in single metal and bimetallic systems suggests that H atom transfer is the dominant mechanism in Fe/Pd system, while e-transfer is still the dominant mechanism in Fe/Ag system.
Показать больше [+] Меньше [-]Dynamic multimedia fate simulation of Perfluorooctane Sulfonate (PFOS) from 1981 to 2050 in the urbanizing Bohai Rim of China
2018
Su, Chao | Lü, Yonglong | Wang, Tieyu | Lu, Xiaotian | Song, Shuai | Li, Lei | Kifāyatullāh, K̲h̲ān | Wang, Chenchen | Liang, Ruoyu
Perfluorooctane sulfonate (PFOS) and related substances are widely used in various industrial and commercial applications in China that ultimately discharge sufficient quantities of PFOS to the environment. It remains unclear how emissions of PFOS ultimately affect its concentrations as well as its fate in the environment. In this study, an improved Berkeley-Trent (BETR) multimedia model is developed to predict the PFOS levels with spatial and temporal distributions on unsteady state mode from 1981 to 2050, by taking the Bohai Rim of China as a case. The results showed that the modeled concentrations agreed well with the measured data. According to the model, PFOS concentrations in fresh water peaked in some months after the peak emission (2008 or 2009), whereas in urban soil the concentrations increased to peak slightly later (around 2014). Among the selected regions, Beijing and Tianjin were simulated with higher PFOS levels in the past and present because of their higher urbanization and industrialization since the 1980s, while in the future, Shandong and Liaoning are expected to have higher concentrations of PFOS than those in Beijing. The water system including coastal water, fresh water and sediment was the biggest sink for PFOS for coastal regions. Among the chemical inputs, direct primary emissions played a more important role, whereas for chemical removal processes, inter-regional advection and background outflow were the predominant pathways. The results would be useful to control the PFOS releases in China and will help the management agencies to implement the “Stockholm Convention” effectively.
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