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Contribution of liquid water content enhancing aqueous phase reaction forming ambient particulate nitrosamines Full text
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 [-]Chemical aging of hydrochar improves the Cd2+ adsorption capacity from aqueous solution Full text
2021
Li, Detian | Cui, Hongbiao | Cheng, Yueqin | Xue, Lihong | Wang, Bingyu | He, Huayong | Hua, Yun | Chu, Qingnan | Feng, Yanfang | Yang, Linzhang
Hydrochar (HC) serves as a promising adsorbent to remove the cadmium from aqueous solution due to porous structure. The chemical aging method is an efficient and easy-operated approach to improve the adsorption capacity of HC. In this study, four chemical aging hydrochars (CAHCs) were obtained by using nitric acid (HNO₃) with mass fractions of 5% (N5-HC), 10% (N10-HC), and 15% (N15-HC) to age the pristine HC (N0-HC) and remove the Cd²⁺ from the aqueous solution. The results displayed that the N15-HC adsorption capacity was 19.99 mg g⁻¹ (initial Cd²⁺ concentration was 50 mg L⁻¹), which increased by 7.4 folds compared to N0-HC. After chemical aging, the specific surface area and oxygen-containing functional groups of CAHCs were increased, which contributed to combination with Cd²⁺ by physical adsorption and surface complexation. Moreover, ion exchange also occurred during the adsorption process of Cd²⁺. These findings have important implications for wastewater treatment to transform the forestry waste into a valuable adsorbent for Cd²⁺ removal from water.
Show more [+] Less [-]Physiological responses of lichens to factorial fumigations with nitric acid and ozone Full text
2012
Riddell, J. | Padgett, P.E. | Nash, T.H. III
This paper addresses the effects of gaseous nitric acid (HNO₃) and ozone (O₃), two important air pollutants, on six lichen species with different morphological, ecological, and biological characteristics. The treatment chambers were set up in a factorial design consisting of control chambers, chambers fumigated with HNO₃, with O₃, and with HNO₃ and O₃, together. Each species showed a different sensitivity to the fumigations, reflecting the physiological variation among species. Our results clearly indicate that HNO₃ is a strong phytotoxin to many lichens, and that O₃ alone has little effect on the measured parameters. The combined fumigation effects of HNO₃ and O₃ were not significantly different from HNO₃ alone.
Show more [+] Less [-]Estimating the extractability of potentially toxic metals in urban soils: A comparison of several extracting solutions Full text
2007
Madrid, F. | Reinoso, R. | Florido, M.C. | Díaz Barrientos, E. | Ajmone-Marsan, F. | Davidson, CM | Madrid, L.
Metals released by the extraction with aqua regia, EDTA, dilute HCl and sequential extraction (SE) by the BCR protocol were studied in urban soils of Sevilla, Torino, and Glasgow. By multivariate analysis, the amounts of Cu, Pb and Zn liberated by any method were statistically associated with one another, whereas other metals were not. The mean amounts of all metals extracted by HCl and by SE were well correlated, but SE was clearly underestimated by HCl. Individual data for Cu, Pb and Zn by both methods were correlated only if each city was considered separately. Other metals gave poorer relationships. Similar conclusions were reached comparing EDTA and HCl, with much lower values for EDTA. Dilute HCl extraction cannot thus be recommended for general use as alternative to BCR SE in urban soils. Dilute HCl extraction is tested as an alternative to the BCR sequential extraction in urban soils.
Show more [+] Less [-]A simple, rapid and accurate method for the sample preparation and quantification of meso- and microplastics in food and food waste streams Full text
2022
Lievens, Siebe | Slegers, Thomas | Mees, Maarten A. | Thielemans, Wim | Poma, Giulia | Covaci, Adrian | Van Der Borght, Mik
Plastics are produced and used in large quantities worldwide (e.g. as food packaging). In line with this, plastic particles are found throughout the ecosphere and in various foods. As a result, plastics are also present in energy-rich waste biomass derived from the food industry, supermarkets, restaurants, etc. These waste streams are a valuable source for biogas production but can also be used to feed insects that in turn upcycle it into new high-value biomass. In both applications, the remaining residue can be used as fertilizer. Due to the present plastic particles, these applications could pose a continued threat to the environment, and both human and animal health. Therefore, the need of determining the (micro)plastic content to assess the potential danger is rising. In this research, a closed-vessel microwave-assisted acid digestion method was developed to accurately determine meso- and microplastic contents in food (waste) matrices by solubilising this food matrix. Polyvinyl chloride (PVC) food packaging foil was used to develop the method, using a full factorial design with three parameters (nitric acid concentration (c(HNO₃)), temperature (T), and time (t)). According to this model, the best practical conditions were c(HNO₃) = 0.50 mol/L, T = 170 °C, and t = 5.00 min. Subsequently, the method was tested on five other plastics, namely high- and low-density polyethylene (HDPE and LDPE), polypropylene (PP), polystyrene (PS), and polyethylene terephthalate (PET), mixed with a food matrix, resulting in a mean plastic recovery of 102.2 ± 4.1%. Additionally, the polymers were not oxidised during the microwave digestion. For PVC and PS hardly any degradation was found, while HDPE, LDPE, and PP showed slight chain degradation, although without recovery loss. In conclusion, the method is an accurate approach to quantify the total meso- and microplastic content in food (waste) matrices with minimal change in their intrinsic characteristics.
Show more [+] Less [-]Nitrogen burden from atmospheric deposition in East Asian oceans in 2010 based on high-resolution regional numerical modeling Full text
2021
Itahashi, Syuichi | Hayashi, Kentaro | Takeda, Shigenobu | Umezawa, Yu | Matsuda, Kazuhide | Sakurai, Tatsuya | Uno, Itsushi
East Asian oceans are possibly affected by a high nitrogen (N) burden because of the intense anthropogenic emissions in this region. Based on high-resolution regional chemical transport modeling with horizontal grid scales of 36 and 12 km, we investigated the N burden into East Asian oceans via atmospheric deposition in 2010. We found a high N burden of 2–9 kg N ha⁻¹ yr⁻¹ over the Yellow Sea, East China Sea (ECS), and Sea of Japan. Emissions over East Asia were dominated by ammonia (NH₃) over land and nitrogen oxides (NOₓ) over oceans, and N deposition was dominated by reduced N over most land and open ocean, whereas it was dominated by oxidized N over marginal seas and desert areas. The verified numerical modeling identified that the following processes were quantitatively important over East Asian oceans: the dry deposition of nitric acid (HNO₃), NH₃, and coarse-mode (aerodynamic diameter greater than 2.5 μm) NO₃⁻, and wet deposition of fine-mode (aerodynamic diameter less than 2.5 μm) NO₃⁻ and NH₄⁺. The relative importance of the dry deposition of coarse-mode NO₃⁻ was higher over open ocean. The estimated N deposition to the whole ECS was 390 Gg N yr⁻¹; this is comparable to the discharge from the Yangtze River to the ECS, indicating the significant contribution of atmospheric deposition. Based on the high-resolution modeling over the ECS, a tendency of high deposition in the western ECS and low deposition in the eastern ECS was found, and a variety of deposition processes were estimated. The dry deposition of coarse-mode NO₃⁻ and wet deposition of fine-mode NH₄⁺ were the main factors, and the wet deposition of fine-mode NO₃⁻ over the northeastern ECS and wet deposition of coarse-mode NO₃⁻ over the southeastern ECS were also found to be significant processes determining N deposition over the ECS.
Show more [+] Less [-]Sensitivity of fine particulate matter concentrations in South Korea to regional ammonia emissions in Northeast Asia Full text
2021
Kim, Eunhye | Kim, Byeong-Uk | Kim, Hyun Cheol | Kim, Soontae
Ammonia (NH₃) is an important precursor for forming PM₂.₅. In this study, we estimated the impact of upwind transboundary and local downwind NH₃ emissions on PM₂.₅ and its inorganic components via photochemical grid model simulations. Nine sensitivity scenarios with ±50% perturbations of upwind (China) and/or downwind (South Korea) NH₃ emissions were simulated for the year 2016 over Northeast Asia. The annual mean PM₂.₅ concentrations in the downwind area were predicted to change from −3.3 (−18%) to 2.4 μg/m3(13%) when the NH₃ emissions in the upwind and downwind areas were perturbed by -50% to +50%. The change in PM₂.₅ concentrations in the downwind area depending on the change in NH₃ emissions in the upwind area was the highest in spring, followed by winter. This was mainly attributed to the change in nitrate (NO₃⁻), a secondary inorganic aerosol (SIA) that is a predominant constituent of PM₂.₅. Since NH₃ is mainly emitted near the surface and vertical mixing is limited during the night, it was modeled that the aloft nitric acid (HNO₃)-to-NO₃⁻ conversion in the morning hours was increased when the NH₃ accumulated near the surface during nighttime begins to mix up within the Planetary Boundary Layer (PBL) as it develops after sunrise. This implies that the control of upwind and/or downwind NH₃ emissions is effective at reducing PM₂.₅ concentrations in the downwind area even under NH₃ rich conditions in Northeast Asia.
Show more [+] Less [-]Wood ash effects on growth and cadmium uptake in Deschampsia flexuosa (Wavy hair-grass) Full text
2019
Kindtler, Nikolaj Lunding | Ekelund, Flemming | Rønn, Regin | Kjøller, Rasmus | Hovmand, Mads | Vestergård, Mette | Christensen, Søren | Johansen, Jesper Liengaard
Wood ash recycling to forests is beneficial because it regains nutrients and prevents acidification, but wood ash application is restricted due to its cadmium (Cd) content. We question if Cd in wood ash represents a problem, since decreases in Cd bioavailability due to ash-induced pH changes may counteract increased total Cd concentration. We studied effects of wood ash (0, 3, 9 and 30 t ha−1) and lime (pH increase equivalent to the wood ash treatments) on growth and Cd uptake in Deschampsia flexuosa. After four months, we measured plant biomass and Cd accumulation, and extracted Cd from the soil using three different methods; HNO3 (total), EDTA (chelator-based) and NH4NO3 (salt-based). Wood ash and lime strongly stimulated plant growth. Cd concentration in the plant tissue decreased with wood ash and lime addition, and correlated positively with the NH4NO3 extractable fraction of Cd in the soil. In contrast, HNO3 and EDTA extracted more Cd with increased wood ash application. We conclude that wood ash amendment increases soil pH, total Cd concentration, nutrient levels and stimulates plant growth. However, it does not increase Cd accumulation in D. flexuosa, as pH-driven decreases in Cd bioavailability leads to reduced plant Cd uptake. Finally, soil bioavailable Cd is best determined using NH4NO3-extraction.
Show more [+] Less [-]Multisurface modeling of Ni bioavailability to wheat (Triticum aestivum L.) in various soils Full text
2018
Zhao, Xiaopeng | Jiang, Yang | Gu, Xueyuan | Gu, Cheng | Taylor, J Anita | Evans, Les J.
Continual efforts have been made to determine a simple and universal method of estimating heavy metal phytoavailability in terrestrial systems. In the present study, a mechanism-based multi-surface model (MSM) was developed to predict the partition of Ni(II) in soil–solution phases and its bioaccumulation in wheat (Triticum aestivum L.) in 19 Chinese soils with a wide range of soil properties. MSM successfully predicted the Ni(II) dissolution in 0.01 M CaCl2 extracting solution (R2 = 0.875). The two-site model for clay fraction improved the prediction, particularly for alkaline soils, because of the additional consideration of edge sites. More crucially, the calculated dissolved Ni(II) was highly correlated with the metal accumulation in wheat (R2 = 0.820 for roots and 0.817 for shoots). The correlation coefficients for the MSM and various chemical extraction methods have the following order: soil pore water > MSM ≈ diffuse gradient technique (DGT) > soil total Ni > 0.43 M HNO3 > 0.01 M CaCl2. The results suggested that the dissolved Ni(II) calculated using MSM can serve as an effective indicator of the bioavailability of Ni(II) in various soils; hence, MSM can be used as an supplement for metal risk prediction and assessment besides chemical extraction techniques.
Show more [+] Less [-]Speciation and reactivity of lead and zinc in heavily and poorly contaminated soils: Stable isotope dilution, chemical extraction and model views Full text
2017
Ren, Zong-ling | Sivry, Yann | Tharaud, Mickaël | Cordier, Laure | Li, Yongtao | Dai, Jun | Benedetti, Marc F.
Correct characterization of metal speciation and reactivity is a prerequisite for the risk assessment and remedial activity management of contaminated soil. To better understand the intrinsic reactivity of Pb and Zn, nine heavily and poorly contaminated soils were investigated using the combined approaches of chemical extractions, multi-element stable isotopic dilution (ID) method, and multi-surface modelling. The ID results show that 0.1–38% of total Pb and 3–45% of total Zn in the studied soils are isotopically exchangeable after a 3-day equilibration. The intercomparison between experimental and modelling results evidences that single extraction with 0.43 M HNO3 solubilizes part of non-isotopically exchangeable fraction of Pb and Zn in the studied soils, and cannot be used as a surrogate for ID to assess labile Pb and Zn pools in soil. Both selective sequential extraction (SSE) and modelling reveal that Mn oxides are the predominant sorption surface for Pb in the studied soils; while Zn is predicted to be mainly associated with soil organic matter in the soil with low pH and Fe/Mn oxides in the soils with high pH. Multi-surface modelling can provide a reasonable prediction of Pb and Zn adsorption onto different soil constituents for the most of the studied soils. The modelling could be a promising tool to decipher the underlying mechanism that controls metal reactivity in soil, but the submodel for Mn oxides should be incorporated and the model parameters, especially for the 2-pK diffuse layer model for Mn oxides, should be updated in the further studies.
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