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Endogenous release of metals with dissolved organic carbon from biochar: Effects of pyrolysis temperature, particle size, and solution chemistry Full text
2019
Hameed, Rashida | Cheng, Leilei | Yang, Kun | Fang, Jing | Lin, Daohui
Metals are released from biochar (BC) in either the free or dissolved organic carbon (DOC)-combined form. The complexation of metals with DOC influences their toxicity and bioavailability in the environment. The endogenous release of metal species with heterogeneous DOC from BC is very complex; this process has been neglected and remains unaddressed in the literature to date. In this study, the yield and chemical properties of labile DOC from BC were characterized, and the release of endogenous metal/metalloid elements (K, Mg, Mn, Fe, Al, Cu, and Si) and their species from BC with various pyrolysis temperatures and particle sizes were systematically investigated under various solution chemistries. The results showed that pyrolysis temperature of BC significantly influenced the yield and composition of DOC and DOC-metal/metalloid complexes, while particle size had lower impact. The yield of BC-derived DOC significantly decreased and the components gradually changed from low-molecular weight and low-aromaticity hydrophilic humic acid-like substances to complex high-molecular weight and high-aromaticity hydrophobic substances as pyrolysis temperature increased from 200 to 700 °C. The release of total dissolved metals decreased with increasing pyrolysis temperature, while the highest total dissolved Si was released from BC with the moderate pyrolysis temperature (500 °C). The metal elements were mainly released in the DOC-combined form, while the released Si was mainly in the free form in the neutral water environment. The release of DOC increased while that of dissolved metals decreased with increasing solution pH. The release of total dissolved metals/metalloids increased but the ratio of the DOC-combined metals/metalloids decreased with increasing solution ionic strength. These results provide new insight into the understanding of endogenous metal/metalloid release from BC in the natural environment.
Show more [+] Less [-]Comparison of long-term stability under natural ageing between cement solidified and chelator-stabilised MSWI fly ash Full text
2019
Du, Bing | Li, Jiantao | Fang, Wen | Liu, Jianguo
Cement-solidification and chelator-stabilisation of municipal solid waste incineration fly ash (MSWI-FA) are two main treatment techniques to immobilise heavy metals. Differences in the long-term stabilities of those two methods of heavy-metal immobilisation were explored to aid in determining the better MSWI-FA treatment. However, few comparative studies have been conducted on 6-year-old cement-solidified FA (Ce-6-FA) and chelator-stabilised FA (Ch-6-FA). In this study, we compared the physicochemical and heavy metal leaching characteristics of Ce-6-FA and Ch-6-FA. The chemical speciation of heavy metals was modelled using geochemical software to assess long-term stability. The results showed weaker long-term stability in Pb immobilisation under the chelating system. The leaching concentrations of target heavy metals, acetic acid leaching tests, acid neutralising capacity, and pH-dependent leaching results indicated that Ce-6-FA had higher long-term stability than Ch-6-FA. A column experiment indicated that the cumulative release rates of Pb in Ce-6-FA and Ch-6-FA were 2.49% and 4.72%, respectively. The phase-controlled leaching of Pb in Ce-6-FA mainly occurred through Pb2(OH)3Cl and chloropyromorphite (Pb5(PO4)3Cl), whereas that in Ch-6-FA mainly occurred through Pb5(PO4)3Cl. The decomposition of heavy metal chelates in Ch-6-FA and salt generation in this process led to the release of Pb via the inorganic complex.
Show more [+] Less [-]Bioturbation effects on metal release from contaminated sediments are metal-dependent Full text
2019
Xie, Minwei | Simpson, Stuart L. | Wang, Wen-Xiong
Metal flux measurements inform the mobility, potential bioavailability and risk of toxicity for metals in contaminated sediments and therefore is an important approach for sediment quality assessment. The binding and release of metals that contribute to the net flux is strongly influenced by the presence and behaviors of benthic organisms. Here we studied the effects of bioturbation on the mobility and efflux of metals from multi-metal contaminated sediments that inhabited by oligochaete worms or both worms and bivalves. Presence of bivalves enhanced the release of Mn, Co, Ni and Zn but not for copper and chromium, which is likely due to the high affinities of copper and chromium for the solid phase. Metals in the overlying water were primarily associated with fractions smaller than 10 kDa, and the fractionation of all metals were not affected by the presence of the bivalve. Metal fluxes attributed to different processes were also distinguished, and the bioturbation induced effluxes were substantially higher than the diffusive effluxes. Temporal variabilities in the total net effluxes of Mn, Co, Ni and Zn were also observed and were attributed to the biological activities of the bivalves. Overall, the present study demonstrated that the response of different metals to the same bioturbation behavior was different, resulting in distinct mobility and fate of the metal contaminants.
Show more [+] Less [-]Climate change has weakened the ability of Chinese lakes to bury polycyclic aromatic hydrocarbons Full text
2019
Tao, Yuqiang | Zhang, Ya | Cao, Jicheng | Wu, Zifan | Yao, Shuchun | Xue, Bin
Burial in sediments is a crucial way to reduce mobilization and risks of hydrophobic organic contaminants (HOCs), but ability of sediments to bury HOCs may be altered if the environment is changed. Whether the ability of sediments to bury HOCs has been affected by climate change remains largely unclear. We excluded the impacts of anthropogenic emissions and eutrophication from that of climate change, and for the first time found that not only the rising surface air temperature but also the declining wind speed and the reducing days with precipitation had weakened the ability of Chinese lakes to bury 16 polycyclic aromatic hydrocarbon (PAHs) by 69.2% ± 9.4%–85.7% ± 3.6% from 1951 to 2017. The relative contributions of the climatic variables to the reduced burial ability depended on the properties of the PAHs, and lakes. Burial ability of the PAHs responded differently to climate change, and was correlated to their volatilization and aqueous solubility, and lake area, catchment area/lake area ratio, and water depth. Our study suggests that not only the rising surface air temperature but also the declining wind speed and the reducing days with precipitation can undermine global efforts to reduce environmental and human exposure to PAHs.
Show more [+] Less [-]Short-term exposure to ambient ozone and inflammatory biomarkers in cross-sectional studies of children and adolescents: Results of the GINIplus and LISA birth cohorts Full text
2019
Zhao, Tianyu | Markevych, Iana | Standl, Marie | Schikowski, Tamara | Berdel, Dietrich | Koletzko, Sibylle | Jörres, Rudolf A. | Nowak, Dennis | Heinrich, Joachim
While exposure to ambient particulate matter (PM) and nitrogen dioxide (NO₂) is thought to be associated with diseases via inflammatory response, the association between exposure to ozone, an oxidative pollutant, and inflammation has been less investigated.We analyzed associations between short-term exposure to ozone and three inflammatory biomarkers among children and adolescents.These cross-sectional analyses were based on two follow-ups of the GINIplus and LISA German birth cohorts. We included 1330 10-year-old and 1591 15-year-old participants. Fractional exhaled nitric oxide (FeNO) and high-sensitivity C-reactive protein (hs-CRP) were available for both age groups while interleukin (IL)-6 was measured at 10 years only. Maximum 8-h averages of ozone and daily average concentrations of NO₂ and PM with an aerodynamic diameter <10 μm (PM₁₀) were adopted from two background monitoring stations 0 (same day), 1, 2, 3, 5, 7, 10 and 14 days prior to the FeNO measurement or blood sampling. To assess associations, we utilized linear regression models for FeNO, and logistic regressions for IL-6 and hs-CRP, adjusting for potential covariates and co-pollutants NO₂ and PM₁₀.We found that short-term ozone exposure was robustly associated with higher FeNO in adolescents at age 15, but not at age 10. No consistent associations were observed between ozone and IL-6 in children aged 10 years. The relationship between hs-CRP levels and ozone was J-shaped. Relatively low ozone concentrations (e.g., <120 μg/m³) were associated with reduced hs-CRP levels, while high concentrations (e.g., ≥120 μg/m³) tended to be associated with elevated levels for both 10- and 15-year-old participants.Our study demonstrates significant associations between short-term ozone exposure and FeNO at 15 years of age and a J-shaped relationship between ozone and hs-CRP. The finding indicates that high ozone exposure may favor inflammatory responses in adolescents, especially regarding airway inflammation.
Show more [+] Less [-]Characterizations of microbial diversity and machine oil degrading microbes in machine oil contaminated soil Full text
2019
Wang, Mengjiao | Deng, Baiwan | Fu, Xun | Sun, Haiyan | Xu, Zhimin
Microbial diversity in machine oil contaminated soil was determined by high-throughput amplicon sequencing technology. The diversity of culturable microbes in the contaminated soil was further characterized using polymerase chain reaction method. Proteobacteria and Bacteroidetes were the most dominant phyla and occupied 52.73 and 16.77%, respectively, while the most abundant genera were Methylotenera (21.62%) and Flavobacterium (3.06%) in the soil. In the culturable microbes, the major phyla were Firmicutes (46.15%) and Proteobacteria (37.36%) and the most abundant genera were Bacillus (42.86%) and Aeromonas (34.07%). Four isolated microbes with high machine oil degradation efficiency were selected to evaluate their characteristics on the oil degradation. All of them reached their highest oil degradation rate after 7 days of incubation. Most of them significantly increased their oil degradation rate by additional carbon or organic nitrogen source in the incubation medium. The oil degradation rate by combination of the four microbes at the same level was also higher than the rate from each individual microbe. The protocol and findings of this study are very useful for developing micro-bioremediation method to eliminate machine oil contaminants from soil.
Show more [+] Less [-]A potential source for PM2.5: Analysis of fine particle generation mechanism in Wet Flue Gas Desulfurization System by modeling drying and breakage of slurry droplet Full text
2019
Jiang, Binfan | Xie, Yulei | Xia, Dehong | Liu, Xiangjun
Aerosol particulate matter with dynamic diameter smaller than 2.5 μm (PM₂.₅) is the main cause for haze pollution in China. As a dominant precursor of PM₂.₅, SO₂ emitted from industrial process is now strictly controlled by using limestone/gypsum Wet Flue Gas Desulfurization (WFGD) system in China. However, a phenomenon that fine particle derived from WFGD is recently addressed, and is suggested to be a potential source of primary PM₂.₅. Herein, a first investigation into the particle generation mechanism in WFGD system is conducted with a novel droplet (containing particles) drying and breakage model. The proposed model considers a random and porous crust instead of the previous regular crust assumption, and is verified by comparing the modeling results with measurements. An orthogonal test with four factors and three levels is carried out through modeling calculation, and flue gas temperature (Tg) in the inlet is found to be a governing parameter for PM₂.₅ yields in WFGD. With Tg in range of 120–160 °C, PM₂.₅ yields in desulfurizing tower can reach a maximum value at ∼2 × 10⁸ cm⁻³ under typical WFGD condition. To avoid this situation and reduce the PM₂.₅ generation, Tg is suggested to be lower than 120 °C. Additionally, a new insight of the elimination effect of gas-gas heater (GGH) on “gypsum rain” in WFGD system is provided.
Show more [+] Less [-]Nanoparticle TiO2 size and rutile content impact bioconcentration and biomagnification from algae to daphnia Full text
2019
Chen, Xiangjie | Zhu, Ya | Yang, Kun | Zhu, Lizhong | Lin, Daohui
Little information is available about effect of particle size and crystal structure of nTiO₂ on their trophic transfer. In this study, 5 nm anatase, 10 nm anatase, 100 nm anatase, 20 nm P25 (80% anatase and 20% rutile), and 25 nm rutile nTiO₂ were selected to investigate the effects of size and crystal structure on the toxicity, bioconcentration, and trophic transfer of nTiO₂ to algae and daphnia. In the exposed daphnids, metabolic pathways affected by nTiO₂ and nTiO₂-exposed algae (nTiO₂-algae) were also explored. The 96 h IC₅₀ values of algae and the 48 h LC₅₀ values of daphnia were 10.3, 18.9, 43.9, 33.6, 65.4 mg/L and 10.5, 13.2, 37.0, 28.4, 60.7 mg/L, respectively, after exposed to nTiO₂-5A, nTiO₂-10A, nTiO₂-100A, nTiO₂-P25, and nTiO₂-25R, respectively. The bioconcentration factors (BCFs) for 0.1, 1, and 10 mg/L nTiO₂ in daphnia ranged from 21,220 L/kg to 145,350 L/kg. The nTiO₂ biomagnification factors (BMFs) of daphnia fed with 1 and 10 mg/L nTiO₂-exposed algae were consistently greater than 1.0 (5.7–122). The results show that the acute toxicity, BCF, and BMF all decreased with increasing size or rutile content of nTiO₂. All types of nTiO₂ were largely accumulated in the daphnia gut and were not completely depurated within 24 h. At the molecular level, 22 Kyoto Encyclopedia of Genes and Genomes (KEGG) metabolic pathways of daphnia were impacted by the nTiO₂ and nTiO₂-algae treatments, including glutathione metabolism, aminoacyl-tRNA biosynthesis, among others. Six and four KEGG metabolic pathways were significantly disturbed in daphnids exposed to nTiO₂ and nTiO₂-algae, respectively, indicating the presence of algae partially alleviated the negative impact of nTiO₂ on metabolism. These findings increase understanding of the impacts of physicochemical properties of nTiO₂ on the food chain from molecular scale to that of the whole organism, and provide new insight into the ecological effect of nanomaterials.
Show more [+] Less [-]Kinetics and mechanism of photocatalytic degradation of methyl orange in water by mesoporous Nd-TiO2-SBA-15 nanocatalyst Full text
2019
High-efficiency nanophotocatalysts with large specific surface areas have a broad range of application prospects in the catalytic oxidation treatment of organic pollutants in wastewater. A chemical method was used to synthesize a TiO₂ nanophotocatalyst with a mesoporous structure upon which a rare earth metal (Nd) was deposited, namely Nd-TiO₂-SBA-15 (NTS). The prepared NTS was characterized using X-ray diffractometry, transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectrometry. The photocatalytic mechanism was explored using scavenger experiments with photoinduced carriers combined with total organic carbon and UV–Vis measurements. At the same time, the kinetic properties of the NTS photocatalytic degradation of methyl orange (MO) were evaluated. The results showed that the deposition of TiO₂ nanoparticles on the surface of the SBA-15 molecular sieve did not change the mesoporous structure, and Nd was uniformly distributed on the surface of the nanophotocatalyst. The photogenerated holes of the NTS played an important role in the photocatalysis process. In addition, the synthesized NTS had good adaptability in the range of pH 2–10. At pH 4, the reaction rate constant (k) of the MO photocatalytic degradation by NTS was 0.011825 mg·(L·min)⁻¹, and the adsorption equilibrium constant (K) was 0.051359 L mg⁻¹. In addition, the photocatalytic degradation rate of MO by NTS remained above 70%, even when the NTS was recycled four times. The NTS showed a good performance after recycling. This work provides a good foundation for the large-scale application of NTS.
Show more [+] Less [-]Nitrogen deposition affects both net and gross soil nitrogen transformations in forest ecosystems: A review Full text
2019
Cheng, Yi | Wang, Jing | Chang, Scott X. | Cai, Zucong | Müller, Christoph | Zhang, Jinbo
Nitrogen (N) deposition has rapidly increased and is influencing forest ecosystem processes and functions on a global scale. Understanding process-specific N transformations, i.e., gross N transformations, in forest soils in response to N deposition is of great significance to gain mechanistic insights on the linkages between global N deposition and N availability or loss in forest soils. In this paper, we review factors controlling N mineralization, nitrification and N immobilization, particularly in relation to N deposition, discuss the limitations of net N transformation studies, and synthesize the literature on the effect of N deposition on gross N transformations in forest ecosystems. We found that more than 97% of published papers evaluating the effect of N deposition (including N addition experiments that simulate N deposition) on soil N cycle determined net rates of mineralization and nitrification, showing that N deposition significantly increased those rates by 24.9 and 153.9%, respectively. However, studies on net N transformation do not provide a mechanistic understanding of the effect of N deposition on N cycling. To date, a small number of studies (<20 published papers) have directly quantified the effect of N deposition on gross N transformation rates, limiting our understanding of the response of soil N cycling to N deposition. The responses to N deposition of specific N transformation processes such as autotrophic nitrification, heterotrophic nitrification, dissimilatory nitrate reduction to ammonium, N mineralization, and N immobilization are poorly studied. Future research needs to use more holistic approaches to study the impact of N deposition on gross N transformation rates, N loss and retention, and their microbial-driven mechanisms to provide a better understanding of the processes involved in N transformations, and to understand the differential responses between forest and other ecosystems.
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