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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.
اظهر المزيد [+] اقل [-]Contrasting exchanges of nitrogen and phosphorus across the sediment–water interface during the drying and re-inundation of littoral eutrophic sediment
2019
Liu, Cheng | Du, Yiheng | Chen, Kaining | Ma, Shuzhan | Chen, Bingfa | Lan, Yuanming
High water level fluctuations (WLFs) lead to periodic drying and re-inundation of sediments in the littoral area of eutrophic lakes. In this study, a series of littoral sediment cores were dried for different periods (5–30 d) and rewetted for 48 h. The sediment cores that dried for 30 d were then re-inundated for 90 d. The exchanges of nitrogen (N) and phosphorus (P) across the sediment–water interface (SWI) and the mechanisms were studied. The results showed that ammonium nitrogen (NH4+–N) fluxes increased after 5–25 d of drying, which was followed by an obvious decrease after 30 d of drying. The decreased NH4+–N fluxes remained at low levels during the 90 d re-inundation period. The soluble reactive P (SRP) fluxes decreased significantly after 15 d of drying. However, further re-inundation increased the SRP fluxes to their initial levels. The decreased water content and porosity, the oxidation of the sediment during drying, and the associated transformations of the N and P fractions in the sediment from drying to re-inundation influenced the exchanges of NH4+–N and SRP across the SWI. The decrease of labile NH4+–N in the sediment during drying was non-reversible, while the transformations between redox sensitive P (Fe-P) and aluminum-bound P were more likely to be reversible from drying to re-inundation. The increase of Fe-P during drying and dissolution of Fe-P during the re-inundation were responsible for the development of SRP fluxes from drying to re-inundation. Therefore, the periodic drying and re-inundation of the littoral eutrophic sediments reduced the release of NH4+–N but accelerated the release of SRP from the sediment. This should be given more consideration for the remediation and management of eutrophication in the lake and other similar lakes with high WLFs.
اظهر المزيد [+] اقل [-]Redox and global interconnected proteome changes in mice exposed to complex environmental hazards surrounding Doñana National Park
2019
Michán, Carmen | Chicano-Gálvez, Eduardo | Fuentes-Almagro, Carlos A. | Alhama, José
Natural environments are receiving an increasing number of contaminants. Therefore, the evaluation and identification of early responses to pollution in these complex habitats is an urgent and challenging task. Doñana National Park (DNP, SW Spain) has been widely used as a model area for environmental studies because, despite its strictly protected core, it is surrounded by numerous threat sources from agricultural, mining and industrial activities. Since many pollutants often induce oxidative stress, redox proteomics was used to detect redox-based variations within the proteome of Mus spretus mice captured in DNP and the surrounding areas. Functional analysis showed that most differentially oxidized proteins are involved in the maintenance of homeostasis, by eliciting mechanisms to respond to toxic substances and oxidative stress, such as antioxidant and biotransformation processes, immune and inflammatory responses, and blood coagulation. Furthermore, changes in the overall protein abundance were also analysed by label-free quantitative proteomics. The upregulation of phase I and II biotransformation enzymes in mice from Lucio del Palacio may be an alert for organic pollution in the area located at the heart of DNP. Metabolic processes involved in protein turnover (proteolysis, amino acid catabolism, new protein biosynthesis and folding) were activated in response to oxidative damage to these biomolecules. Consequently, aerobic respiratory metabolism increased to address the greater ATP demands. Alterations of cholesterol metabolism that could cause hepatic steatosis were also detected. The proteomic detection of globally altered metabolic and physiological processes offers a complete view of the main biological changes caused by environmental pollution in complex habitats.
اظهر المزيد [+] اقل [-]Electrocatalytical oxidation of arsenite by reduced graphene oxide via in-situ electrocatalytic generation of H2O2
2019
Li, Xuheng | Liu, Feng | Zhang, Weifang | Lü, Hongbo | Zhang, Jing
Preoxidation of As(III) to As(V) is required for the efficient removal of total arsenic in the treatment of wastewater. In this work, the electro-Fenton oxidation of As(III) with a high efficiency was successfully achieved by using the system of the stainless steel net (SSN) coating with reduced graphene oxide (RGO@SSN) as the cathode and stainless steel net (SSN) as the sacrificial anode. The RGO@SSN was synthesized by electrophoretic deposition-annealing method. The carbon disorder and defects of RGO resulted from the remained oxygen-containing functional groups facilitated the electrocatalytically active sites for two-electron oxygen reduction reaction (ORR). A high concentration (up to 1000 μmol/L) of H₂O₂ was in-situ produced through two-electron oxygen reduction reaction of electro-catalysis, and then served as the electro-Fenton reagent for the oxidation of As(III). HO generated by H₂O₂ participating the electro-Fenton reaction or decomposed at the surface of RGO@SSN cathode at acid condition endowed the strong oxidizing ability for As(III). The electro-Fenton equipped with RGO@SSN cathode has a promising application in the oxidation and removal of organic or inorganic pollutants in wastewater.
اظهر المزيد [+] اقل [-]Origin and properties of soluble brown carbon in freshly emitted and aged ambient aerosols over an urban site in India
2019
Sarakāra, Cirantana | Venkataraman, Chandra | Yadav, Suman | Phuleria, Harish C. | Chatterjee, Abhijit
This work investigates the absorption properties of soluble brown carbon (BrC), extracted in methanol and water, from ambient aerosol (PM₁₀) samples, collected over an urban background site in Mumbai, India. The diurnal variability was investigated in samples collected in the morning (7–11 a.m.) and afternoon (12–4 p.m.) periods. Absorption properties of BrC (in the 300–600-nm wavelength range) were measured in filter extracts of water-soluble organic carbon (WSOC) and methanol-soluble organic carbon (MSOC). WSOC and MSOC accounted for on average 52% and 77%, respectively, of the measured OC, potentially indicating unextracted BrC and rendering these values the lower bound. Compared with afternoon samples, the morning samples of MSOC and WSOC had increased BrC concentrations and absorption coefficients (bₐbₛ365; 40%–65%). The correlation between bₐbₛ365 and EC, ns-K⁺, and NO₃⁻ in the morning samples indicated contributions from primary sources, including both biomass and vehicular sources. The decreased bₐbₛ365 in the afternoon samples was partly explained by mixing layer dilution, accompanied by a reduction in the concentrations of primary aerosol constituents. Furthermore, in the afternoon samples, ¹HNMR spectroscopy revealed the presence of more oxidized functional groups and significantly higher OC/EC and WSOC/OC ratios, indicating the greater aging of afternoon aerosol. The MAC₃₆₅ (m²gC⁻¹) for both WSOC and MSOC extracts decreased significantly by 20%–34% in the afternoon samples compared with the morning samples, indicating degradation in the absorption properties of the particles and potentially a change in the constituent BrC chromophores.
اظهر المزيد [+] اقل [-]Aromatic acids as biomass-burning tracers in atmospheric aerosols and ice cores: A review
2019
Wan, Xin | Kawamura, Kimitaka | Ram, Kirpa | Kang, Shichang | Loewen, Mark | Gao, Shaopeng | Wu, Guangming | Fu, Pingqing | Zhang, Yanlin | Bhattarai, Hemraj | Cong, Zhiyuan
Biomass burning (BB) is one of the largest sources of carbonaceous aerosols with adverse impacts on air quality, visibility, health and climate. BB emits a few specific aromatic acids (p-hydroxybenzoic, vanillic, syringic and dehydroabietic acids) which have been widely used as key indicators for source identification of BB-derived carbonaceous aerosols in various environmental matrices. In addition, measurement of p-hydroxybenzoic and vanillic acids in snow and ice cores have revealed the historical records of the fire emissions. Despite their uniqueness and importance as tracers, our current understanding of analytical methods, concentrations, diagnostic ratios and degradation processes are rather limited and scattered in literature. In this review paper, firstly we have summarized the most established methods and protocols for the measurement of these aromatic acids in aerosols and ice cores. Secondly, we have highlighted the geographical variability in the abundances of these acids, their diagnostic ratios and degradation processes in the environments. The review of the existing data indicates that the concentrations of aromatic acids in aerosols vary greatly with locations worldwide, typically more abundant in urban atmosphere where biomass fuels are commonly used for residential heating and/or cooking purposes. In contrast, their concentrations are lowest in the polar regions which are avoid of localized emissions and largely influenced by long-range transport. The diagnostic ratios among aromatic acids can be used as good indicators for the relative amounts and types of biomass (e.g. hardwood, softwood and herbaceous plants) as well as photochemical oxidation processes. Although studies suggest that the degradation processes of the aromatic acids may be controlled by light, pH and hygroscopicity, a more careful investigation, including closed chamber studies, is highly appreciated.
اظهر المزيد [+] اقل [-]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.
اظهر المزيد [+] اقل [-]Nanotechnology in remediation of water contaminated by poly- and perfluoroalkyl substances: A review
2019
Zhang, Weilan | Zhang, Tongqing | Liang, Yanna
This article gives an overview of nanotechnologies applied in remediation of water contaminated by poly- and perfluoroalkyl substances (PFASs). The use of engineered nanomaterials (ENMs) in physical sorption and photochemical reactions offers a promising solution in PFAS removal because of the high surface area and the associated high reactivities of the ENMs. Modification of carbon nanotubes (CNTs) (e.g., oxidation, applying electrochemical assistance) significantly improves their adsorption rate and capacity for PFASs removal and opens a new door for use of CNTs in environmental remediation. Modified nanosized iron oxides with high adsorption capacity and magnetic property have also been demonstrated to be ideal sorbents for PFASs with great recyclability and thus provide an excellent alternative for PFAS removal under various conditions. Literature shows that PFOA, which is one of the most common PFASs detected at contaminated sites, can be effectively decomposed in the presence of either TiO₂-based, Ga₂O₃-based, or In₂O₃-based nano-photocatalysts under UV irradiation. The decomposition abilities and mechanisms of different nano-photocatalysts are reviewed and compared in this paper. Particularly, the nanosized In₂O₃ photocatalysts have the best potential in PFOA decomposition and the decomposition performance is closely related to the specific surface area and the amount of photogenerated holes on the surfaces of In₂O₃ nanostructures. In addition to detailed review of the published studies, future prospects of using nanotechnology for PFAS remediation are also discussed in this article.
اظهر المزيد [+] اقل [-]Bacterial diversity in typical abandoned multi-contaminated nonferrous metal(loid) tailings during natural attenuation
2019
Liu, Jian-li | Yao, Jun | Wang, Fei | Min, Ning | Gu, Ji-hai | Li, Zi-fu | Sunahara, Geoffrey | Duran, Robert | Solevic-Knudsen, Tatjana | Hudson-Edwards, K. A. (Karen A.) | Alakangas, Lena
Abandoned nonferrous metal(loid) tailings sites are anthropogenic, and represent unique and extreme ecological niches for microbial communities. Tailings contain elevated and toxic content of metal(loid)s that had negative effects on local human health and regional ecosystems. Microbial communities in these typical tailings undergoing natural attenuation are often very poorly examined. The diversity and inferred functions of bacterial communities were examined at seven nonferrous metal(loid) tailings sites in Guangxi (China), which were abandoned between 3 and 31 years ago. The acidity of the tailings sites rose over 31 years of site inactivity. Desulfurivibrio, which were always coupled with sulfur/sulfide oxidation to dissimilate the reduction of nitrate/nitrite, were specific in tailings with 3 years abandonment. However, genus beneficial to plant growth (Rhizobium), and iron/sulfur-oxidizing bacteria and metal(loid)-related genera (Acidiferrobacter and Acidithiobacillus) were specific within tailings abandoned for 23 years or more. The increased abundance of acid-generating iron/sulfur-oxidizing and metal(loid)-related bacteria and specific bacterial communities during the natural attenuation could provide new insights for understanding microbial ecosystem functioning in mine tailings. OTUs related to Sulfuriferula, Bacillus, Sulfurifustis, Gaiella, and Thiobacillus genera were the main contributors differentiating the bacterial communities between the different tailing sites. Multiple correlation analyses between bacterial communities and geochemical parameters indicated that pH, TOC, TN, As, Pb, and Cu were the main drivers influencing the bacterial community structures. PICRUSt functional exploration revealed that the main functions were related to DNA repair and recombination, important functions for bacterial adaptation to cope with the multi-contamination of tailings. Such information provides new insights to guide future metagenomic studies for the identification of key functions beyond metal-transformation/resistance. As well, our results offers novel outlooks for the management of bacterial communities during natural attenuation of multi-contaminated nonferrous metal(loid) tailings sites.
اظهر المزيد [+] اقل [-]Peroxymonosulfate catalyzed by rGO assisted CoFe2O4 catalyst for removing Hg0 from flue gas in heterogeneous system
2019
Zhao, Yi | Nie, Guoxin | Ma, Xiaoying | Xu, Peiyao | Zhao, Xiaochu
The cobalt ferrite-reduced oxidized graphene (CoFe2O4/rGO) catalyst was synthesized by hydrothermal method and characterized by Powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Scanning electron microscope (SEM), Brunauere Emmette Teller (BET) and Hysteresis loop. For developing a new method of removing elemental mercury (Hg0) from flue gas, the effects of catalyst dosage, PMS concentration, solution pH and reaction temperature on the removal efficiency were investigated experimentally by using peroxymonosulfate (PMS) catalyzed by CoFe2O4/rGO at a self-made bubbling reactor. The average removal efficiency of Hg0 in a 30-min period reached 95.56%, when CoFe2O4/rGO dosage was 0.288 g/L, PMS concentration was 3.5 mmol/L, solution pH was 5.5 and reaction temperature was 55 °C. Meanwhile, based on the free radical quenching experiments, in which, ethyl alcohol and tert butyl alcohol were used as quenchers to prove indirectly the presence of •OH and SO4•−, the characterizations of catalysts and reaction products, and the existing results from other scholars. The reaction mechanism was proposed.
اظهر المزيد [+] اقل [-]