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Contribution of liquid water content enhancing aqueous phase reaction forming ambient particulate nitrosamines
2022
Choi, Na Rae | Park, Seungshik | Ju, Seoryeong | Lim, Yong Bin | Lee, Ji Yi | Kim, Eunhye | Kim, Soontae | Shin, Hye Jung | Kim, Yong Pyo
Contribution of liquid water content (LWC) to the levels of the carcinogenic particulate nitro(so) compounds and the chemistry affecting LWC were investigated based on the observation of seven nitrosamines and two nitramines in rural (Seosan) and urban (Seoul) area in South Korea during October 2019 and a model simulation. The concentrations of both the total nitrosamines and nitramines were higher in Seosan (12.48 ± 16.12 ng/m³ and 0.65 ± 0.71 ng/m³, respectively) than Seoul (7.41 ± 13.59 ng/m³ and 0.24 ± 0.15 ng/m³, respectively). The estimated LWC using a thermodynamic model in Seosan (12.92 ± 9.77 μg/m³) was higher than that in Seoul (6.20 ± 5.35 μg/m³) mainly due to higher relative humidity (75 ± 9% (Seosan); 62 ± 10% (Seoul)) and higher concentrations of free ammonia (0.13 ± 0.09 μmol/m³ (Seosan); 0.08 ± 0.01 μmol/m³ (Seoul)) and total nitric acid (0.09 ± 0.07 μmol/m³ (Seosan); 0.04 ± 0.02 μmol/m³ (Seoul)) in Seosan while neither fog nor rain occurred during the sampling period. The relatively high concentrations of the particulate nitrosamines (>30 ng/m³) only observed probably due to the higher LWC (>10 μg/m³) in Seosan. It implies that aqueous phase reactions involving NO₂ and/or uptake from the gas phase enhanced by LWC could be promoted in Seosan. Strong correlation between the concentrations of nitrosodi-methylamine (NDMA), an example of nitrosamines, simulated by a kinetic box model including the aqueous phase reactions and the measured concentration of NDMA in Seosan (R = 0.77; 0.37 (Seoul)) indicates that the aqueous phase reactions dominantly enhanced the NDMA concentrations in Seosan. On the other hand, it is estimated that the formation of nitrosamines by aqueous phase reaction was not significant due to the relatively lower LWC in Seoul compared to that in Seosan. Furthermore, it is presumed that nitramines are mostly emitted from the primary emission sources. This study implies that the concentration of the particulate nitrosamines can be promoted by aqueous phase reaction enhanced by LWC.
Show more [+] Less [-]Phase-specific stable isotope fractionation effects during combined gas-liquid phase exchange and biodegradation
2022
Khan, Ali M. | Gharasoo, Mehdi | Wick, Lukas Y. | Thullner, Martin
Stable isotope fractionation of toluene under dynamic phase exchange was studied aiming at ascertaining the effects of gas-liquid partitioning and biodegradation of toluene stable isotope composition in liquid-air phase exchange reactors (Laper). The liquid phase consisted of a mixture of aqueous minimal media, a known amount of a mixture of deuterated (toluene-d) and non-deuterated toluene (toluene-h), and bacteria of toluene degrading strain Pseudomonas putida KT2442. During biodegradation experiments, the liquid and air-phase concentrations of both toluene isotopologues were monitored to determine the observable stable isotope fractionation in each phase. The results show a strong fractionation in both phases with apparent enrichment factors beyond −800‰. An offset was observed between enrichment factors in the liquid and the gas phase with gas-phase values showing a stronger fractionation in the gas than in the liquid phase. Numerical simulation and parameter fitting routine was used to challenge hypotheses to explain the unexpected experimental data. The numerical results showed that either a very strong, yet unlikely, fractionation of the phase exchange process or a – so far unreported – direct consumption of gas phase compounds by aqueous phase microorganisms could explain the observed fractionation effects. The observed effect can be of relevance for the analysis of volatile contaminant biodegradation using stable isotope analysis in unsaturated subsurface compartments or other environmental compartment containing a gas and a liquid phase.
Show more [+] Less [-]Facile nanoplastics formation from macro and microplastics in aqueous media
2022
Peller, Julie R. | Mezyk, Stephen P. | Shidler, Sarah | Castleman, Joe | Kaiser, Scott | Faulkner, Richard F. | Pilgrim, Corey D. | Wilson, Antigone | Martens, Sydney | Horne, Gregory P.
The immense production of plastic polymers combined with their discordancy with nature has led to vast plastic waste contamination across the geosphere, from the oceans to freshwater reservoirs, wetlands, remote snowpacks, sediments, air and multiple other environments. These environmental pollutants include microplastics (MP), typically defined as small and fragmented plastics less than 5 mm in size, and nanoplastics (NP), particles smaller than a micrometer. The formation of micro and nanoplastics in aqueous media to date has been largely attributed to fragmentation of plastics by natural (i.e., abrasion, photolysis, biotic) or industrial processes. We present a novel method to create small microplastics (≲ 5 μm) and nanoplastics in water from a wide variety of plastic materials using a small volume of a solubilizer liquid, such as n-dodecane, in combination with vigorous mixing. When the suspensions or solutions are subjected to ultrasonic mixing, the particle sizes decrease. Small micro- and nanoparticles were made from commercial, real world and waste (aged) polyethylene, polystyrene, polycarbonate and polyethylene terephthalate, in addition to other plastic materials and were analyzed using dark field microscopy, Raman spectroscopy and particle size measurements. The presented method provides a new and simple way to create specific size distributions of micro- and nanoparticles, which will enable expanded research on these plastic particles in water, especially those made from real world and aged plastics. The ease of NP and small MP formation upon initial mixing simulates real world environments, thereby providing further insight into the behavior of plastics in natural settings.
Show more [+] Less [-]Application of gas chromatographic retention times to determine physicochemical properties of nitrated, oxygenated, and parent polycyclic aromatic hydrocarbons
2022
Vuong, Quang Tran | Son, Ji-Min | Thang, Phan Quang | Ohura, Takeshi | Choi, Sung-Deuk
Nitrated and oxygenated polycyclic aromatic hydrocarbons (NPAHs and OPAHs) are receiving attention because of their high toxicity compared with parent PAHs. However, the experimental data of their physicochemical properties has been limited. This study proposed the gas chromatographic retention time (GC-RT) technique as an effective alternative one to determine octanol-air partition coefficients (KOA) and sub-cooled liquid vapor pressures (PL) for 11 NPAHs, 10 OPAHs, and 19 parent PAHs. The slopes and intercepts of the linear regressions between temperature versus KOA and PL were provided and can be used to estimate KOA and PL for the 40 targeted compounds at any temperature. The internal energies of phase transfer (ΔUOA) and enthalpies of vaporization (ΔHL) for all targeted compounds were also calculated using the GC-RT technique. High-molecular-weight compounds may release or absorb higher heat energy to transform between different phases. NPAHs and OPAHs had a non-ideal solution behavior with activity in octanol (γₒcₜ) in the range of 19–53 and 18–1,078, respectively, which is larger than the unity threshold. A comparison among four groups of PAH derivatives showed that a functional group (nitro-, oxygen-, chloro-, and bromo-) in PAH derivatives increased γₒcₜ for corresponding parent PAHs by tens (mono-group) to hundreds of times (di-group). This study suggests that the GC-RT method is applicable for indirectly measuring the physicochemical properties of various groups of organic compounds.
Show more [+] Less [-]Thermal processing reduces PFAS concentrations in blue food – A systematic review and meta-analysis
2022
Vendl, Catharina | Pottier, Patrice | Taylor, Matthew D. | Bräunig, Jennifer | Gibson, Matthew J. | Hesselson, Daniel | Neely, G Gregory | Lagisz, Malgorzata | Nakagawa, Shinichi
Per- and polyfluoroalkyl substances (PFAS) are ubiquitous in the environment and often ingested with food. PFAS exposure in people can have detrimental health consequences. Therefore, reducing PFAS burdens in food items is of great importance to public health. Here, we investigated whether cooking reduces PFAS concentrations in animal-derived food products by synthesizing experimental studies. Further, we examined the moderating effects of the following five variables: cooking time, liquid/animal tissue ratio, cooking temperature, carbon chain length of PFAS and the cooking category (oil-based, water-based & no-liquid cooking). In our systematic review searches, we obtained 512 effect sizes (relative differences in PFAS concentration between raw and cooked samples) from 10 relevant studies. These studies exclusively explored changes in PFAS concentrations in cooked seafood and freshwater fish. Our multilevel-meta-analysis has revealed that, on average, cooking reduced PFAS concentrations by 29%, although heterogeneity among effect sizes was very high (I² = 94.65%). Our five moderators cumulatively explained 49% of the observed heterogeneity. Specifically, an increase in cooking time and liquid/animal tissue ratio, as well as shorter carbon chain length of PFAS (when cooked with oil) were associated with significant reductions in PFAS concentrations. The effects of different ways of cooking depended on the other moderators, while the effect of cooking temperature itself was not significant. Overall, cooking can reduce PFAS concentrations in blue food (seafood and freshwater fish). However, it is important to note that complete PFAS elimination requires unrealistically long cooking times and large liquid/animal tissue ratios. Currently, literature on the impact of cooking of terrestrial animal produce on PFAS concentrations is lacking, which limits the inference and generalisation of our meta-analysis. However, our work represents the first step towards developing guidelines to reduce PFAS in food via cooking exclusively with common kitchen items and techniques.
Show more [+] Less [-]Underwater noise emissions from ships during 2014–2020
2022
Jalkanen, Jukka-Pekka | Johansson, Lasse | Andersson, Mathias H. | Majamäki, Elisa | Sigray, Peter
This paper reports trends in the input of underwater noise source energy emission from global shipping, based on bottom-up modeling of individual ships. In terms of energy, we predict the doubling of global shipping noise emissions every 11.5 years, on average, but there are large regional differences. Shipping noise emissions increase rapidly in Arctic areas and the Norwegian Sea. The largest contributors are the containerships, dry bulk and liquid tanker vessels which emit 75% of the underwater shipping noise source energy. The COVID-19 pandemic changed vessel traffic patterns and our modeling indicates a reduction of −6% in global shipping noise source energy in the 63 Hz ⅓ octave band. This reduction was largest in the Greenland Sea, the Coastal Waters of Southeast Alaska and British Columbia as well as the Gulf of California, temporarily disrupting the increasing pre-pandemic noise emission trend. However, in some sea areas, such as the Indian Ocean, Yellow Sea and Eastern China Sea the emitted noise source energy was only slightly reduced. In global scale, COVID-19 pandemic reduced the underwater shipping noise emissions close to 2017 levels, but it is expected that the increasing trend of underwater noise emissions will continue when the global economy recovers.
Show more [+] Less [-]Secondary inorganic aerosol chemistry and its impact on atmospheric visibility over an ammonia-rich urban area in Central Taiwan
2022
Young, Li-Hao | Hsiao, Ta-Chih | Griffith, Stephen M. | Huang, Yaxin | Hsieh, Hao-Gang | Lin, Tang-Huang | Tsay, Si-Chee | Lin, Yu-Jung | Lai, Kuan-Lin | Lin, Neng-Huei | Lin, Wen-Yinn
This study investigated the hourly inorganic aerosol chemistry and its impact on atmospheric visibility over an urban area in Central Taiwan, by relying on measurements of aerosol light extinction, inorganic gases, and PM₂.₅ water-soluble ions (WSIs), and simulations from a thermodynamic equilibrium model. On average, the sulfate (SO₄²⁻), nitrate (NO₃⁻), and ammonium (NH₄⁺) components (SNA) contributed ∼90% of WSI concentrations, which in turn made up about 50% of the PM₂.₅ mass. During the entire observation period, PM₂.₅ and SNA concentrations, aerosol pH, aerosol liquid water content (ALWC), and sulfur and nitrogen conversion ratios all increased with decreasing visibility. In particular, the NO₃⁻ contribution to PM₂.₅ increased, whereas the SO₄²⁻ contribution decreased, with decreasing visibility. The diurnal variations of the above parameters indicate that the interaction and likely mutual promotion between NO₃⁻ and ALWC enhanced the hygroscopicity and aqueous-phase reactions conducive for NO₃⁻ formation, thus led to severely impaired visibility. The high relative humidity (RH) at the study area (average 70.7%) was a necessary but not sole factor leading to enhanced NO₃⁻ formation, which was more directly associated with elevated ALWC and aerosol pH. Simulations from the thermodynamic model depict that the inorganic aerosol system in the study area was characterized by fully neutralized SO₄²⁻ (i.e. a saturated factor in visibility reduction) and excess NH₄⁺ amidst a NH₃-rich environment. As a result, PM₂.₅ composition was most sensitive to gas-phase HNO₃, and hence NOx, and relatively insensitive to NH₃. Consequently, a reduction of NOx would result in instantaneous cuts of NO₃⁻, PM₂.₅, and ALWC, and hence improved visibility. On the other hand, a substantial amount of NH₃ reduction (>70%) would be required to lower the aerosol pH, driving more than 50% of the particulate phase NO₃⁻ to the gas phase, thereby making NH₃ a limiting factor in shifting PM₂.₅ composition.
Show more [+] Less [-]PCDD/Fs and heavy metals in the vicinity of landfill used for MSWI fly ash disposal: Pollutant distribution and environmental impact assessment
2022
Lin, Xiaoqing | Ma, Yunfeng | Chen, Tong | Wang, Lei | Takaoka, Masaki | Pan, Shuping | Zhang, Hao | Wu, Angjian | Li, Xiaodong | Yan, Jianhua
This study focused on the syngenetic control of polychlorinated-ρ-dibenzodioxins and dibenzofurans (PCDD/Fs) and heavy metals by field stabilization/solidification (S/S) treatment for municipal solid waste incineration fly ash (MSWIFA) and multi-step leachate treatment. Modified European Community Bureau of Reference (BCR) speciation analysis and risk assessment code (RAC) revealed the medium environment risk of Cd and Mn, indicating the necessity of S/S treatment for MSWIFA. S/S treatment significantly declined the mass/toxic concentrations of PCDD/Fs (i.e., from 7.21 to 4.25 μg/kg; from 0.32 to 0.20 μg I-TEQ/kg) and heavy metals in MSWIFA due to chemical fixation and dilution effect. The S/S mechanism of sodium dimethyldithiocarbamate (SDD) and cement was decreasing heavy metals in the mild acid-soluble fraction to reduce their mobility and bioavailability. Oxidation treatment of leachate reduced the PCDD/F concentration from 49.10 to 28.71 pg/L (i.e., from 1.60 to 0.98 pg I-TEQ/L) by suspension absorption or NaClO oxidation decomposition, whereas a so-called “memory effect” phenomena in the subsequent procedures (adsorption, press filtration, flocculating settling, slurry separation, and carbon filtration) increased it back to 38.60 pg/L (1.66 pg I-TEQ/L). Moreover, the multi-step leachate treatment also effectively reduced the concentrations of heavy metals to 1–4 orders of magnitude lower than the national emission standards. Furthermore, the PCDD/Fs and heavy metals in other multiple media (soil, landfill leachate, groundwater, and river water) and their spatial distribution characteristics site were also investigated. No evidence showed any influence of the landfill on the surrounding liquid media. The slightly higher concentration of PCDD/Fs in the soil samples was ascribed to other waste management processes (transportation and unloading) or other local source (hazardous incineration plant). Therefore, proper management of landfills and leachate has a negligible effect on the surrounding environment.
Show more [+] Less [-]Bioimmobilization of lead in phosphate mining wasteland by isolated strain Citrobacter farmeri CFI-01
2022
Li, Yizhong | Guo, Shuyu | Zheng, Yunting | Yu, Junxia | Chi, Ruan | Xiao, Chunqiao
Industrial phosphate rock (PR) treatment has introduced lead (Pb) contamination into phosphate mining wasteland, causing serious contamination. Although bioremediation is considered an effective method and studies have investigated the bioimmobilization of Pb contamination in phosphate mining wasteland by phosphate-solubilizing bacteria (PSB), the bioimmobilization mechanism remains unclear. In this study, a strain Citrobacter farmeri CFI-01 with phosphate-solubilizing and Pb-tolerant abilities was isolated from a phosphate mining wasteland. Liquid culture experiments showed that the maximum content of soluble phosphate and the percentage amount of Pb immobilized after 14 days were 351.5 mg/L and 98.18%, respectively, with a decrease in pH. Soil experiments showed that CFI-01 had reasonable bioimmobilization ability, and the percentage amount of Pb immobilized was increased by 7.790% and 22.18% in the groups inoculated with CFI-01, respectively, compared with that of the groups not inoculated with CFI-01. Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), and scanning electron microscopy (SEM) analyses showed that the immobilization of Pb was also ascribed to changes in the functional groups (e.g., hydroxyl and carboxyl groups) and the formation of lead phosphate sediments. Finally, the results of the metagenomic analysis indicated that changes in the microbial community structure, enrichment of related functional abundances (e.g., metal metabolism, carbohydrate metabolism, and amino acid metabolism functions), and activation of functional genes (e.g., zntA, smtB, cadC, ATOX1, smtA, and ATX1) could help immobilize soil Pb contamination and explore the mechanism of bacterial bioimmobilization in Pb-contaminated soil. This study provides insights for exploring the immobilization mechanism of Pb contamination in phosphate mining wasteland using PSB, which has significance for further research.
Show more [+] Less [-]Activation of peroxydisulfate by ball-milled α-FeOOH/biochar composite for phenol removal: Component contribution and internal mechanisms
2022
Zhao, Ling | Zhang, Hui | Zhao, Beibei | Lyu, Honghong
Persulfate-based advanced oxidation process is considered as a promising technology for the degradation of phenol, where efficient, cost effective, and green methods with high peroxydisulfate (PS) activation capacity is of increasing demand. In this work, an in-situ liquid phase precipitation combined with ball milling method was applied for the synthesized of α-FeOOH/biochar, as be the PS activator for phenol degradation. Results showed that the ball-milled α-FeOOH and red pine wood biochar prepared at 700 °C (BM-α-FeOOH/PBC700) exhibited the highest catalytic property with PS for phenol oxidation (a phenol removal rate of 100%), compared with the BM-α-FeOOH (16.0%) and BMPBC700 (66.3%). The presence of intermediate products such as hydroquinone and catechol, and total organic carbon (TOC) removal rate (88.9%) proved the oxidation of phenol in the BM-α-FeOOH/PBC700+PS system. The characterization results showed that the functional groups (e.g., CO, C–O, Fe–O, and Si–O), the dissolved organic matter (DOM) in biochar, the loading of Fe element, and higher degree of graphitization and defect structures, contributed to the activation of PS to form free radicals (i.e., SO₄·⁻, ·OH, ·O₂⁻, and hVB⁺) for phenol oxidation, of which, SO₄·⁻ and ·OH account for 72.1% of the phenol removal rate. The specific contribution to the PS activation for phenol oxidation by each part of the materials was calculated based on the “whole to part” experiment. The contribution of DOM, acid-soluble substance, and carbon matrix and basal part in BM-α-FeOOH/PBC700 were 6.0%, 40.9%, and 53.1%, respectively. The reusability experiments of BM-α-FeOOH/PBC700 demonstrated that the composite was relatively stable after four cycles of reuse. Among three co-existing anions (NO₃⁻, Cl⁻, and HCO₃⁻), HCO₃⁻ played the most significant inhibition effects on phenol removal through reducing the phenol removal rate from 89.6% to 77.9%. This work provides guidance for the design of high active and stable carbon materials that activate PS to remove phenol.
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