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Chemical transformation of CO2 during its capture by waste biomass derived biochars Full text
2016
Xu, Xiaoyun | Kan, Yue | Zhao, Ling | Cao, Xinde
Biochar is a porous carbonaceous material with high alkalinity and rich minerals, making it possible for CO2 capture. In this study, biochars derived from pig manure, sewage sludge, and wheat straw were evaluated for their CO2 sorption behavior. All three biochars showed high sorption abilities for CO2, with the maximum capacities reaching 18.2–34.4 mg g−1 at 25 °C. Elevating sorption temperature and moisture content promoted the transition of CO2 uptake from physical to chemical process. Mineral components such as Mg, Ca, Fe, K, etc. in biochar induced the chemical sorption of CO2 via the mineralogical reactions which occupied 17.7%–50.9% of the total sorption. FeOOH in sewage sludge biochar was transformed by sorbed CO2 into Fe(OH)2CO3, while the sorbed CO2 in pig manure biochar was precipitated as K2Ca(CO3)2 and CaMg(CO3)2, which resulted in a dominant increase of insoluble inorganic carbon in both biochars. For wheat straw biochar, sorbed CO2 induced CaCO3 transformed into soluble Ca(HCO3)2, which led to a dominant increase of soluble inorganic carbons. The results obtained from this study demonstrated that biochar as a unique carbonaceous material could distinctly be a promising sorbent for CO2 capture in which chemical sorption induced by mineralogical reactions played an important role.
Show more [+] Less [-]Influence of temperature on phenanthrene toxicity towards nitrifying bacteria in three soils with different properties Full text
2016
Suszek-Łopatka, Beata | Maliszewska-Kordybach, Barbara | Klimkowicz-Pawlas, Agnieszka | Smreczak, Bożena
This study focused on the combined effect of environmental conditions (temperature) and contamination (polycyclic aromatic hydrocarbons, PAHs) on the activity of soil microorganisms (nitrifying bacteria). Phenanthrene (Phe) at five contamination levels (0, 1, 10, 100 and 1000 mg kg−1 dry mass of soil) was employed as a model PAH compound in laboratory experiments that were conducted at three temperatures (i.e., 20 °C (recommended by ISO 15685 method), 15 and 30 °C). Three soils with different properties were used in these studies, and the activity of the nitrifying bacteria was assessed based on nitrification potential (NP) determinations. For the statistical evaluation of the results, the ANCOVA (analysis of covariance) method for three independent variables (i.e., temperature, phenanthrene concentration, soil matrix (as a qualitative variable)) and their interactions was employed. The results indicated on the significant interaction of all studied factors. Temperature influenced the toxicity of Phe towards NP, and this effect was related to the Phe concentration as well as was varied for the different soils. A low content of soil organic matter (controlling bioavailability of phenanthrene to soil microorganisms) enhanced the combined effect of temperature and Phe toxicity, and a high biological activity of the soil (high NP values) increased the effect of high temperature on the Phe stimulatory influence. The results indicate that the temperature should not be neglected in tests evaluating PAH ecotoxicity, especially for reliable ecological risk assessment.
Show more [+] Less [-]Characterization and source apportionment of volatile organic compounds based on 1-year of observational data in Tianjin, China Full text
2016
Liu, Baoshuang | Liang, Danni | Yang, Jiamei | Dai, Qili | Bi, Xiaohui | Feng, Yinchang | Yuan, Jie | Xiao, Zhimei | Zhang, Yufen | Xu, Hong
From November 2014 to October 2015, the concentrations of volatile organic compounds (VOCs), O3 and NOx were simultaneously monitored by using online instruments at the air monitoring station belonged to Tianjin Environmental Protection Bureau (TEPB). The results indicated that VOCs concentrations were higher in autumn and lower in spring, while O3 concentrations were higher in summer, and lower in winter. The diurnal variations of VOCs and NOx (NO2 plus NO) showed opposite tendency comparing to that of O3. The concentrations of alkanes were higher (the average of 18.2 ppbv) than that of aromatics (5.3 ppbv) and alkenes (5.2 ppbv), however, the alkenes and aromatics made larger contributions to ozone because of their high reactivity. Tianjin belonged to the VOC-limited region during most of seasons (except summer) according to the VOC/NOx ratios (the 8:1 threshold). The automobile exhaust, industrial emission, liquefied petroleum gas/natural gas (LPG/NG), combustion, gasoline evaporation, internal combustion engine emission and solvent usage were identified as major sources of VOCs by Positive Matrix Factorization (PMF) model in Tianjin, and the contributions to VOCs for the entire year were 23.1%, 19.9%, 18.6%, 10.6%, 8.7%, 5.4% and 4.7%, respectively. The conditional probability function (CPF) analysis indicated that the contributing directions of automobile exhaust and industrial emission were mainly affected by source distributions, and that of other sources might be mainly affected by wind direction. The backward trajectory analysis indicated that the trajectory of air mass originated from Mongolia, which reflected the features of large-scale and long-distance air transport, and that of beginning in Jiangsu, Shandong and Tianjin, which showed the features of small-scale and short-distance. Tianjin, Beijing, Hebei and Northwest of Shandong were identified as major potential source-areas of VOCs by using potential source contribution function (PSCF) and concentration-weighted trajectory (CWT) models.
Show more [+] Less [-]Evolution of secondary inorganic and organic aerosols during transport: A case study at a regional receptor site Full text
2016
Peng, Jianfei | Hu, Min | Gong, Zhaoheng | Tian, Xudong | Wang, Ming | Zheng, Jing | Guo, Qingfeng | Cao, Wei | Lv, Wei | Hu, Weiwei | Wu, Zhijun | Guo, Song
Understanding the evolution of aerosols in the atmosphere is of great importance for improving air quality and reducing aerosol-related uncertainties in global climate simulations. Here, a unique haze episode at a regional receptor site near the East China Sea was examined as a case study of the aging process of atmospheric aerosols during transport. An increase in photochemical age from 5 h to more than 25 h and a progressive increase in the fitted mean particle diameter from 70 nm to approximately 300 nm were observed. According to the pollution features and meteorology conditions involved, pollution accumulation (PA), sea breeze (SB), and land breeze (LB) periods were identified. Concentrations of black carbon (BC), hydrocarbon-like organic aerosols (HOA), semi-volatile oxidized organic aerosols (SV-OOA), and nitrate increased by 7-fold up to 39-fold when the air masses passed through Taizhou, a nearby city. In addition, nitrate and SV-OOA dominated the aerosol composition in the urban outflow plumes (52% and 18%, respectively), yet they gradually decreased in concentration during transport. In contrast, sulfate and the low-volatile oxidized organic aerosols (LV-OOA) exhibited more regional footprints and potentially have similar formation mechanisms. The atomic oxygen-to-carbon (O/C) ratio also increased from 0.45 to 0.9, thereby suggesting that rapid formation of highly oxidized secondary organic aerosols (SOA) occurred during transport. Overall, these results provide valuable insight into the evolution of the chemical and physical features of aerosol pollution during transport and also highlight the need for regulatory controls of nitrogen oxides, sulfur dioxide, and VOCs to improve air quality on different scales.
Show more [+] Less [-]Evidence of immunocompetence reduction induced by cadmium exposure in honey bees (Apis mellifera) Full text
2016
Polykretis, P. | Delfino, G. | Petrocelli, I. | Cervo, R. | Tanteri, G. | Montori, G. | Perito, B. | Branca, J.J.V. | Morucci, G. | Gulisano, M.
In the last decades a dramatic loss of Apis mellifera hives has been reported in both Europe and USA. Research in this field is oriented towards identifying a synergy of contributing factors, i.e. pathogens, pesticides, habitat loss and pollution to the weakening of the hive. Cadmium (Cd) is a hazardous anthropogenic pollutant whose effects are proving to be increasingly lethal. Among the multiple damages related to Cd contamination, some studies report that it causes immunosuppression in various animal species. The aim of this paper is to determine whether contamination by Cd, may have a similar effect on the honey bees’ immunocompetence. Our results, obtained by immune challenge experiments and confirmed by structural and ultrastructural observations show that such metal causes a reduction in immunocompetence in 3 days Cd exposed bees. As further evidence of honey bee response to Cd treatment, Energy Dispersive X-ray Spectroscopy (X-EDS) has revealed the presence of zinc (Zn) in peculiar electron-dense granules in fat body cells. Zn is a characteristic component of metallothioneins (MTs), which are usually synthesized as anti-oxidant and scavenger tools against Cd contamination. Our findings suggest that honey bee colonies may have a weakened immune system in Cd polluted areas, resulting in a decreased ability in dealing with pathogens.
Show more [+] Less [-]Combined analysis of trace elements and isotopic composition of particulate organic matter in suspended sediment to assess their origin and flux in a tropical disturbed watershed Full text
2016
Fernandes, Alexandre Martins | Hissler, Christophe | da Conceição, Fabiano Tomazini | Spatti Junior, Eder Paulo | Mortatti, Jefferson
Approximately 40% of the volume of domestic sewage generated in the São Paulo State is untreated and released into water bodies, causing serious pollution problems that affect the water quality and especially the suspended sediments transported by rivers. Thus, this paper investigates the seasonal influence on the origin and fluxes of Cu, Co, Cr, Zn, Cd, Ni, Sc and particulate organic matter (POM) in sediments transported by a disturbed watershed in the São Paulo State, i.e. the Sorocaba River basin. POM was characterized using particulate organic carbon, particulate organic nitrogen, C:N ratio and δ13C and δ15N stable isotopic composition. Eight sample collections of fine suspended sediments (FSS) were carried out at the mouth of the Sorocaba River from July 2009 to May 2010. During the study period, the discharge rate followed the seasonal variation trend of the past 25 years. Zn was the most abundant trace element in the FSS, followed by Cr, Cu, Ni, Co, Sc and Cd. There was a higher concentration of trace elements during the dry season, except for Sc and Co, which did not vary seasonally. The POM showed the same trend, with higher concentrations during the dry season. The calculated enrichment factors and geoaccumulation index indicated that most of the trace elements are of geogenic origin, except for Zn, which showed significant anthropogenic contributions (55%). The elemental and isotopic analysis of C and N and C:N ratio indicated that the anthropogenic origin of POM found in the FSS is related mainly to domestic sewage (97%), while the significant correlation found between the concentrations of Zn and POM indicates that the main anthropogenic source of Zn is related to this domestic sewage. The FSS load transported during the study period was of 373,194 t y−1, of which 87% occurred during the rainy season.
Show more [+] Less [-]Reconstructing temporal variation of fluoride uptake in eastern grey kangaroos (Macropus giganteus) from a high-fluoride area by analysis of fluoride distribution in dentine Full text
2016
Kierdorf, Horst | Rhede, Dieter | Death, Clare | Hufschmid, Jasmin | Kierdorf, Uwe
Trace element profiling in the incrementally formed dentine of mammalian teeth can be applied to reconstruct temporal variation of incorporation of these elements into the tissue. Using an electron microprobe, this study analysed fluoride distribution in dentine of first and third mandibular molars of free-ranging eastern grey kangaroos inhabiting a high-fluoride area, to assess temporal variation in fluoride uptake of the animals. Fluoride content in the early-formed dentine of first molars was significantly lower than in the late-formed dentine of these teeth, and was also lower than in both, the early and the late-formed dentine of third molars. As early dentine formation in M1 takes place prior to weaning, this finding indicates a lower dentinal fluoride uptake during the pre-weaning compared to the post-weaning period. This is hypothetically attributed to the action of a partial barrier to fluoride transfer from blood to milk in lactating females and a low bioavailability of fluoride ingested together with milk. Another factor contributing to lower plasma fluoride levels in juveniles compared to adults is the rapid clearance of fluoride from blood plasma in the former due to their intense skeletal growth. The combined action of these mechanisms is considered to explain why in kangaroos from high-fluoride areas, the (early-formed) first molars are not affected by dental fluorosis while the (later-formed) third and fourth molars regularly exhibit marked to severe fluorotic lesions.
Show more [+] Less [-]Rate constants of hydroxyl radical oxidation of polychlorinated biphenyls in the gas phase: A single−descriptor based QSAR and DFT study Full text
2016
Yang, Zhihui | Luo, Shuang | Wei, Zongsu | Ye, Tiantian | Spinney, Richard | Chen, Dong | Xiao, Ruiyang
The second‒order rate constants (k) of hydroxyl radical (·OH) with polychlorinated biphenyls (PCBs) in the gas phase are of scientific and regulatory importance for assessing their global distribution and fate in the atmosphere. Due to the limited number of measured k values, there is a need to model the k values for unknown PCBs congeners. In the present study, we developed a quantitative structure–activity relationship (QSAR) model with quantum chemical descriptors using a sequential approach, including correlation analysis, principal component analysis, multi−linear regression, validation, and estimation of applicability domain. The result indicates that the single descriptor, polarizability (α), plays an important role in determining the reactivity with a global standardized function of lnk = −0.054 × α ‒ 19.49 at 298 K. In order to validate the QSAR predicted k values and expand the current k value database for PCBs congeners, an independent method, density functional theory (DFT), was employed to calculate the kinetics and thermodynamics of the gas‒phase ·OH oxidation of 2,4′,5-trichlorobiphenyl (PCB31), 2,2′,4,4′-tetrachlorobiphenyl (PCB47), 2,3,4,5,6-pentachlorobiphenyl (PCB116), 3,3′,4,4′,5,5′-hexachlorobiphenyl (PCB169), and 2,3,3′,4,5,5′,6-heptachlorobiphenyl (PCB192) at 298 K at B3LYP/6–311++G**//B3LYP/6–31 + G** level of theory. The QSAR predicted and DFT calculated k values for ·OH oxidation of these PCB congeners exhibit excellent agreement with the experimental k values, indicating the robustness and predictive power of the single–descriptor based QSAR model we developed.
Show more [+] Less [-]A century long sedimentary record of anthropogenic lead (Pb), Pb isotopes and other trace metals in Singapore Full text
2016
Chen, Mengli | Boyle, Edward A. | Switzer, Adam D. | Gouramanis, Chris
Reconstructing the history of metal deposition in Singapore lake sediments contributes to understanding the anthropogenic and natural metal deposition in the data-sparse Southeast Asia. To this end, we present a sedimentary record of Pb, Pb isotopes and eleven other metals (Ag, As, Ba, Cd, Co, Cr, Cu, Ni, Tl, U and Zn) from a well-dated sediment core collected near the depocenter of MacRitchie Reservoir in central Singapore. Before the 1900s, the sedimentary Pb concentration was less than 2 mg/kg for both soil and sediment, with a corresponding 206Pb/207Pb of ∼1.20. The Pb concentration increased to 55 mg/kg in the 1990s, and correspondingly the 206Pb/207Pb decreased to less than 1.14. The 206Pb/207Pb in the core top sediment is concordant with the 206Pb/207Pb signal of aerosols in Singapore and other Southeast Asian cities, suggesting that Pb in the reservoir sediment was mainly from atmospheric deposition. Using the Pb concentration in the topmost layer of sediment, the estimated atmospheric Pb flux in Singapore today is ∼1.6 × 10−2 g/m2 yr. The concentrations of eleven other metals preserved in the sediment were also determined. A principal component analysis showed that most of the metals exhibit an increasing trend towards 1990s with a local concentration peak in the mid-20th century.
Show more [+] Less [-]Effects of conventional and biodegradable microplastics on a marine ecosystem engineer (Arenicola marina) and sediment nutrient cycling Full text
2016
Green, Dannielle Senga | Boots, Bas | Sigwart, Julia | Jiang, Shan | Rocha, Carlos
Effects of microplastic pollution on benthic organisms and ecosystem services provided by sedimentary habitats are largely unknown. An outdoor mesocosm experiment was done to realistically assess the effects of three different types of microplastic pollution (one biodegradable type; polylactic acid and two conventional types; polyethylene and polyvinylchloride) at increasing concentrations (0.02, 0.2 and 2% of wet sediment weight) on the health and biological activity of lugworms, Arenicola marina (Linnaeus, 1758), and on nitrogen cycling and primary productivity of the sediment they inhabit. After 31 days, A. marina produced less casts in sediments containing microplastics. Metabolic rates of A. marina increased, while microalgal biomass decreased at high concentrations, compared to sediments with low concentrations or without microplastics. Responses were strongest to polyvinylchloride, emphasising that different materials may have differential effects. Each material needs to be carefully evaluated in order to assess their risks as microplastic pollution. Overall, both conventional and biodegradable microplastics in sandy sediments can affect the health and behaviour of lugworms and directly or indirectly reduce primary productivity of these habitats.
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