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Hexachloroethane dechlorination in sulfide-containing aqueous solutions catalyzed by nitrogen-doped carbon materials
2021
Liu, Na | Hu, Qing | Wang, Chao | Tong, Lizhi | Weng, Chih-Huang | Ding, Longzhen
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The kₒbₛ values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid. Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
اظهر المزيد [+] اقل [-]Preparation of biochar-interpenetrated iron-alginate hydrogel as a pH-independent sorbent for removal of Cr(VI) and Pb(II)
2021
Zhao, Chenhao | Hu, Linlin | Zhang, Changai | Wang, Shengsen | Wang, Xiaozhi | Huo, Zhongyang
Herein, a pH-independent interpenetrating polymeric networks (Fe-SA-C) were fabricated from graphitic biochar (BC) and iron-alginate hydrogel (Fe-SA) for removal of Cr(VI) and Pb(II) in aqueous solution. Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy and scanning electron microscope (SEM) results demonstrated that graphitic BC interpenetration increased surface porosity and distorted surfaces of Fe-SA, which boosted availability of hydroxyl (-OH) group. Fe³⁺ as a cross-linking agent of the alginate endowed Fe-SA-C with positive surfaces (positive zeta potential) and excellent pH buffering capacity, while excessive Fe³⁺ was soldered on Fe-SA-C matrix as FeO(OH) and Fe₂O₃. Cr(VI) removal at pH of 3 by Fe-SA-C (20.3 mg g⁻¹) were 30.3% and 410.6% greater than that by Fe-SA and BC, respectively. Fe-SA-C exhibited minor pH dependence over pH range of 2–7 towards Cr(VI) retention. Greater zeta potential of Fe-SA-C over Fe-SA conferred a better electrostatic attraction with Cr(VI). FTIR and XPS of spent sorbents confirmed the reduction accounted for 98.5% for Cr(VI) removal mainly due to participation of –OH. Cr(VI) reduction was further favored by conductive carbon matrix in Fe-SA-C, as evidenced by more negative Tafel corrosion potential. Reductively formed Cr(III) was subsequently complexed with carboxylic groups originating from oxidation of –OH. Thus, Cr(VI) removal invoked electrostatic attraction, reduction, and surface complexation mechanisms. Pb(II) removal with excellent pH independence was mainly ascribed to surface complexation and possible precipitation. Thus, the functionalized, conductive, and positively-charged Fe-SA-C extended its applicability for Cr(VI) and Pb(II) removal from aqueous solutions in a wide pH range. This research could expand the application of hydrogel materials for removal of both cationic and anionic heavy metals in solutions over an extended pH range.
اظهر المزيد [+] اقل [-]Improving denitrification efficiency in constructed wetlands integrated with immobilized bacteria under high saline conditions
2021
Wang, Xinyi | Zhu, Hui | Yan, Baixing | Shutes, B. (Brian) | Bañuelos, Gary | Wen, Huiyang | Cheng, Rui
Constructed wetlands (CWs) inoculated with exogenous microbes have great potential for removing pollutants in adverse environments. The rapid loss of functional bacteria and the high cost of repeated additions of inoculum, however, limit the practical application of this technology. In this study, C–F2 immobilized bacteria (i.e., immobilized salt-tolerant bacterium Alishewanella sp. F2 incorporated with a carbon source) were developed and utilized in CWs for solving the above problems. A 60-day experiment demonstrated that bioaugmented CWs (Bio-CWs) with the addition of C–F2 immobilized bacteria into the bottom gravel layer of CW microcosms (B-CF2 treatment) exhibited high nitrogen removal efficiency under a saline condition (electrical conductivity of 15 mS/cm). We measured mean nitrate nitrogen (NO₃⁻-N) and total nitrogen (TN) removal percentages of 97.8% and 88.1%, respectively, which were significantly (p < 0.05) higher than those in Bio-CWs with microbial inoculum (MI-F2 treatment, 63.5% and 78.2%) and unbioaugmented CWs (CK, 48.7% and 67.2%). The TN content of the entire plant was significantly (p < 0.05) increased in B-CF2 (636.06 mg/microcosm) compared with CK (372.06 mg/microcosm). The relative abundances of the genera Alishewanella (i.e., the exogenous bacterium, 5.5%), Clostridium-XlVa (8.8%) and Bacteroides (21.1%) in B-CF2 were significantly (p < 0.05) higher than in MI-F2 and CK, which improved the denitrification capacity of CWs. Overall, a high denitrification efficiency and durability were achieved in the newly developed Bio-CWs (i.e., B-CF2 treatment) with immobilized bacteria under saline conditions, which provides an alternative technology for the rapid removal of nitrogen from saline wastewater.
اظهر المزيد [+] اقل [-]Factors affecting the exposure to physicochemical and microbiological pollutants in vehicle cabins while commuting in Lisbon
2021
Buitrago, N.D. | Savdie, J. | Almeida, S.M. | Verde, S Cabo
Commuters are exposed to a variety of physicochemical and microbiological pollutants that can lead to adverse health effects. This study aims to evaluate the indoor air quality (IAQ) in cars, buses and trains in Lisbon, to estimate inhaled doses while commuting and to evaluate the impacts of cleaning and ventilation on the IAQ. Particulate matter with diameter lower than 1, 2.5 and 10 μm (PM₁, PM₂.₅ and PM₁₀), black carbon (BC), carbon monoxide (CO), carbon dioxide (CO₂) volatile organic compounds (VOCs), formaldehyde (CH₂O) and total airborne bacteria and fungi were measured and bacterial isolates were identified. Results showed that the type of ventilation is the main factor affecting the IAQ in vehicle cabins. Under the fan off condition, the concentration of BC was lower, but the concentration of gases such as CO₂, CO and VOC tended to accumulate rapidly. When the ventilation was used, the coarse particles were filtered originating the decrease of indoor concentrations. Commuters travelling in trains received the lowest dose for all chemical pollutants, except VOC, mainly because railways are further away from the direct vehicular emissions. Commuters travelling in cars without ventilation received the highest inhaled dose for almost all pollutants despite having the lowest travel duration. Airborne microbiota was highly affected by the occupancy of the vehicles and therefore, the fungi and bacterial loads were higher in trains and buses. Most of the isolated species were human associated bacteria and some of the most abundant species have been linked to respiratory tract infections.
اظهر المزيد [+] اقل [-]Plastic pollution impacts on marine carbon biogeochemistry
2021
Galgani, Luisa | Loiselle, Steven A.
One of the major challenges in understanding the dynamics of the ocean’s health and functioning is the potential impact of the increasing presence of plastic. Besides the verified and macroscopic effects on marine wildlife and habitats, micro and macroplastics offer potential sites for microbial activity and chemical leaching. Most marine plastic is found initially in the upper meters of the water column, where fundamental biogeochemical processes drive marine productivity and food web dynamics. However, recent findings show a continuum of potential effects of these new marine components on carbon, nutrients and microbial processes. In the present analysis, we develop a common ground between these studies and we identify knowledge gaps where new research efforts should be focused, to better determine potential feedbacks of plastics on the carbon biogeochemistry of a changing ocean.
اظهر المزيد [+] اقل [-]Effect of C/N substrates for enhanced extracellular polymeric substances (EPS) production and Poly Cyclic Aromatic Hydrocarbons (PAHs) degradation
2021
Premnath, N. | Mohanrasu, K. | Guru Raj Rao, R. | Dinesh, G.H. | Siva Prakash, G. | Pugazhendhi, Arivalagan | Jeyakanthan, J. | Govarthanan, Muthusamy | Kumar, Ponnuchamy | Arun, A.
Extracellular Polymeric Substances (EPS) influenced Poly Cyclic Aromatic Hydrocarbons (PAHs) degrading Klebsiella pneumoniae was isolated from the marine environment. To increase the EPS production by Klebsiella pneumoniae, several physicochemical parameters were tweaked such as different carbon sources (arabinose, glucose, glycerol, lactose, lactic acid, mannitol, sodium acetate, starch, and sucrose at 20 g/L), nitrogen sources (ammonium chloride, ammonium sulphate, glycine, potassium nitrate, protease peptone and urea at 2 g/L), different pH, carbon/nitrogen ratio, temperature, and salt concentration were examined. Maximum EPS growth and biodegradation of Anthracene (74.31%), Acenaphthene (67.28%), Fluorene (62.48%), Naphthalene (57.84%), and mixed PAHs (55.85%) were obtained using optimized conditions such as glucose (10 g/L) as carbon source, potassium nitrate (2 g/L) as the nitrogen source at pH 8, growth temperature of 37 °C, 3% NaCl concentration and 72 h incubation period. The Klebsiella pneumoniae biofilm architecture was studied by confocal laser scanning microscopy (CLSM) and scanning electron microscope (SEM). The present study demonstrates the EPS influenced PAHs degradation of Klebsiella pneumoniae.
اظهر المزيد [+] اقل [-]Conversion and transformation of N species during pyrolysis of wood-based panels: A review
2021
Xu, Deliang | Yang, Liu | Zhao, Ming | Zhang, Jinrui | Syed Shatir A. Syed-Hassan, | Sun, Hongqi | Hu, Xun | Zhang, Hong | Zhang, Shu
Understanding the migration and conversion of nitrogen in wood-based panels (WBPs) during pyrolysis is fundamentally important for potentially transforming the N-containing species into valuable material-based products. This review firstly summarizes the commonly used methods for examining N evolution during the WBPs pyrolysis before probing into the association between the wood and adhesives.The potential effects of wood-adhesive interaction on the pyrolysis process are subsequently analyzed. Furthermore, the controversial statements from literature on the influence of adhesives on wood pyrolysis behavior are discussed, which is followed by the detailed investigation into the distribution and evolution of N-containing species in gas, liquid and char, respectively, during WBPs pyrolysis in recent studies. The differences in N species due to the heating sources (i.e. electrical heating vs microwave heating) are particularly compared. Finally, based on the characteristics of staged pyrolysis, co-pyrolysis and catalytic pyrolysis, the converting pathways for WBPs are proposed with an emphasis on the production of value-added chemicals and carbon materials, simultaneously mitigating NOₓ emission.
اظهر المزيد [+] اقل [-]Vertical profile of aerosols in the Himalayas revealed by lidar: New insights into their seasonal/diurnal patterns, sources, and transport
2021
Xiang, Yan | Zhang, Tianshu | Liu, Jianguo | Wan, Xin | Loewen, Mark | Chen, Xintong | Kang, Shichang | Fu, Yibin | Lv, Lihui | Liu, Wenqing | Cong, Zhiyuan
Atmospheric aerosols play a crucial role in climate change, especially in the Himalayas and Tibetan Plateau. Here, we present the seasonal and diurnal characteristics of aerosol vertical profiles measured using a Mie lidar, along with surface black carbon (BC) measurements, at Mt. Qomolangma (QOMS), in the central Himalayas, in 2018–2019. Lidar-retrieved profiles of aerosols showed a distinct seasonal pattern of aerosol loading (aerosol extinction coefficient, AEC), with a maximum in the pre-monsoon (19.8 ± 22.7 Mm⁻¹ of AEC) and minimum in the summer monsoon (7.0 ± 11.2 Mm⁻¹ of AEC) seasons. The diurnal variation characteristics of AEC and BC were quite different in the non-monsoon seasons with enriched aerosols being maintained from 00:00 to 10:00 in the pre-monsoon season. The major aerosol types at QOMS were identified as background, pollution, and dust aerosols, especially during the pre-monsoon season. The occurrence of pollution events influenced the vertical distribution, seasonal/diurnal patterns, and types of aerosols. Source contribution of BC based on the weather research and forecasting chemical model showed that approximately 64.2% ± 17.0% of BC at the QOMS originated from India and Nepal in South Asia during the non-monsoon seasons, whereas approximately 47.7% was from local emission sources in monsoon season. In particular, the high abundance of BC at the QOMS in the pre-monsoon season was attributed to biomass burning, whereas anthropogenic emissions were the likely sources during the other seasons. The maximum aerosol concentration appeared in the near-surface layer (approximately 4.3 km ASL), and high concentrations of transported aerosols were mainly found at 4.98, 4.58, 4.74, and 4.88 km ASL in the pre-monsoon, monsoon, post-monsoon, and winter seasons, respectively. The investigation of the vertical profiles of aerosols at the QOMS can help verify the representation of aerosols in the air quality model and satellite products and regulate the anthropogenic disturbance over the Tibetan Plateau.
اظهر المزيد [+] اقل [-]Paper product production identified as the main source of per- and polyfluoroalkyl substances (PFAS) in a Norwegian lake: Source and historic emission tracking
2021
Langberg, Håkon A. | Arp, Hans Peter H. | Breedveld, Gijs D. | Slinde, Gøril A. | Høiseter, Åse | Grønning, Hege M. | Jartun, Morten | Rundberget, Thomas | Jenssen, Bjørn M. | Hale, Sarah E.
The entirety of the sediment bed in lake Tyrifjorden, Norway, is contaminated by per- and polyfluoroalkyl substances (PFAS). A factory producing paper products and a fire station were investigated as possible sources. Fire station emissions were dominated by the eight carbon perfluoroalkyl sulfonic acid (PFSA), perfluorooctanesulfonic acid (PFOS), from aqueous film forming foams. Factory emissions contained PFOS, PFOS precursors (preFOS and SAmPAP), long chained fluorotelomer sulfonates (FTS), and perfluoroalkyl carboxylic acids (PFCA). Concentrations and profiles in sediments and biota indicated that emissions originating from the factory were the main source of pollution in the lake, while no clear indication of fire station emissions was found. Ratios of linear-to branched-PFOS increased with distance from the factory, indicating that isomer profiles can be used to trace a point source. A dated sediment core contained higher concentrations in older sediments and indicated that two different PFAS products have been used at the factory, referred to here as Scotchban and FTS mixture. Modelling, based on the sediment concentrations, indicated that 42–189 tons Scotchban, and 2.4–15.6 tons FTS mixture, were emitted. Production of paper products may be a major PFAS point source, that has generally been overlooked. It is hypothesized that paper fibres released from such facilities are important vectors for PFAS transport in the aquatic environment.
اظهر المزيد [+] اقل [-]Deep winter intrusions of urban black carbon into a canyon near Santiago, Chile: A pathway towards Andean glaciers
2021
Huneeus, Nicolás | Lapere, Rémy | Mazzeo, Andrea | Ordóñez Morales, César Eduardo | Donoso, Nicolás | Munoz, Ricardo | Rutllant, José A.
Black carbon transport from the Santiago Metropolitan Area, Chile, up to the adjacent Andes Cordillera and its glaciers is of major concern. Its deposition accelerates the melting of the snowpack, which could lead to stress on water supply in addition to climate feedback. A proposed pathway for this transport is the channelling through the network of canyons that connect the urban basin to the elevated summits, as suggested by modelling studies, although no observations have validated this hypothesis so far. In this work, atmospheric measurements from a dedicated field campaign conducted in winter 2015, under severe urban pollution conditions, in Santiago and the Maipo canyon, southeast of Santiago, are analysed. Wind (speed and direction) and particulate matter concentrations measured at the surface and along vertical profiles, demonstrate intrusions of thick layers (up to 600 m above ground) of urban black carbon deep into the canyon on several occasions. Transport of PM down-valley occurs mostly through shallow layers at the surface except in connection with deep valley intrusions, when a secondary layer in altitude with return flow (down-valley) at night is observed. The transported particulate matter is mostly from the vicinity of the entrance to the canyon and uncorrelated to concentrations observed in downtown Santiago. Reanalyses data show that for 10% of the wintertime days, deep intrusions into the Maipo canyon are prevented by easterly winds advecting air pollutants away from the Andes. Also, in 23% of the cases, intrusions proceed towards a secondary north-eastward branch of the Maipo canyon, leaving 67% of the cases with favourable conditions for deep penetrations into the main Maipo canyon. Reanalyses show that the wind directions associated to the 33% anomalous cases are related to thick cloud cover and/or the development of coastal lows.
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