Search

Phosphate addition is commonly applied to remediate lead contaminated sites via the formation of lead phosphate particles with low solubility. However, the effects of natural organic matter (NOM) with different properties, as well as the contributions of specific interactions (particle-particle, particle-NOM, and NOM-NOM) in enhanced stabilization or flocculation of the particles, are not currently well understood. This study investigates the influence of two aquatic NOM and two soil or coal humic acid (HA) extracts on the aggregation behavior of lead phosphate particles and explores the controlling mechanisms. All types of NOM induced disaggregation and steric stabilization of the particles in the presence of Na + (100 mM) or low (1 mM) Ca 2+ concentrations, as well as at low NOM concentrations (1 mg C /L). However, for the soil and coal HA, a threshold at NOM concentrations of 10 mg C /L and high (3 mM) Ca 2+ concentrations was observed where bridging flocculation (rather than steric stabilization) occurred. In situ attenuated total reflectance - Fourier transform infrared characterization confirmed adsorption of the soil and coal humic acid extracts (10 mg C /L) onto the surface of the lead phosphate particles in 3 mM Ca 2+ , whereas dynamic and static light scattering demonstrated extensive HA flocculation that dominated the overall scattered light intensities. These results imply that the accelerated aggregation was induced by a combination of HA adsorption and bridging flocculation by Ca 2+ . Overall, this research demonstrates that the type of NOM is critical to predict the colloidal stability of lead phosphate particles. Aquatic NOM stabilized the particles under all conditions evaluated, but soil or coal HA with higher molecular weight and aromaticity showed highly variable stabilization or flocculation behavior depending on the HA and Ca 2+ concentrations available to adsorb to the particles and participate in bridging. These results provide new mechanistic insights on particle stabilization or destabilization by NOM., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Magnetite nanoparticles (MNPs) with varied organic coatings (OCs) which improved their stability have broad environmental applications. However, the adsorbed amounts and layer thickness of varied OCs onto MNPs during the synthesis were generally not or poorly characterized, and their interactions with natural organic matter (NOM) were still in progress. In this study, acetic (HAc), citric (CA), and polyacrylic acid (PAA) were selected as model OCs, the adsorption behaviors of OCs on MNPs were characterized under varied aqueous C/Fe ratios, and the aggregation behaviors of MNPs with varied OCs (OC-MNPs) at neutral pH (7.0 ± 0.2) with NaCl (5-800 mM) in the presence/absence of NOM were systematically investigated. Under low aqueous C/Fe ratio, the adsorbed amounts of model OCs as -COOH/Fe ratio followed the order: CA ≈ PAA > > HAc. With high aqueous C/Fe ratio, the maximum adsorbed masses of OC-MNPs were similar. The adsorbed layer thicknesses of OC-MNPs were thoroughly characterized using three different methods, all showing that the adsorbed layer of PAA was thicker than that of CA and HAc. Derjaguin-Landau-Verwey-Overbeek (DLVO) and extended DLVO (EDLVO) calculations showed that electrostatic and van der Waals forces were dominant for CA-MNPs and HAc-MNPs stabilization; while steric repulsion played major roles in stabilizing PAA-MNPs, probably due to a thicker PAA layer. In the presence of NOM, stability behaviors of all OC-MNPs were similar, ascribing to the much greater amounts of NOM adsorbed than the OCs, causing greater steric repulsion. This study provides new mechanistic insights which could help better understand the effects of varied OCs on MNPs' colloidal stability., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships with other people organizations that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

To enhance the long-term immobilization of radioactive wastes, ferrihydrite nanoparticles were incorporated into cementitious materials. The effects of ferrihydrite nanoparticles on the physicochemical and mechanical properties of cementitious materials and the immobilization of uranium (U), strontium (Sr) and cesium (Cs) were investigated. Adding ferrihydrite nanoparticles at 0.65%, 1.30%, 3.90% and 6.50% of cement weight slightly improved compressive strength by 5-11%, but dramatically reduced U leaching by 50-57%. The enhanced U immobilization was attributed to the strong adsorption of U by ferrihydrite nanoparticles, and the structural incorporation of U into hematite formed during ferrihydrite recrystallization. Although ferrihydrite nanoparticles had weaker effect than hematite nanoparticles on improving cement hydration and reducing permeability, they exhibit stronger U immobilization capacity. In contrast, incorporating ferrihydrite nanoparticles into cementitious materials had no significant effects on Cs and Sr leaching and no detectable adsorption of Sr and Cs. This study elucidated the fundamental differences in the interactions between ferrihydrite nanoparticles and U, Sr or Cs within cementitious systems that led to the distinctive immobilization mechanisms for these radionuclides. It generated new mechanistic understandings of U, Sr and Cs leaching from cementitious barriers modified by Fe-based nanoparticles, and proposed a new approach for enhancing long-term immobilization of U., (Copyright © 2019 Elsevier B.V. All rights reserved.)

To better understand the fate and transport of ferrihydrite nanoparticles (FNPs), which carry many contaminants in natural and engineered aquatic environments, the aggregation of FNPs was systematically investigated in this study. The pH isoelectric point (pH IEP ), surface zeta potential, and particle size evolutions of FNPs were measured under varied aqueous conditions using dynamic light scattering (DLS). The influence of pH (5.0 ± 0.1 and 7.0 ± 0.1), ionic strength (IS), electrolytes (NaCl, CaCl 2 and Na 2 SO 4 ), and organics (humic acid, fulvic acid and CH 3 COONa) on the aggregation behaviors of FNPs were explored. Meanwhile, Derjaguin-Landau-Verwey-Overbeek (DLVO) theory was employed to better understand the controlling mechanisms of FNP aggregation. In the presence of sulfate, the surface charge of FNPs was neutralized under varied pH and ionic strength due to ion adsorption and FNPs phase transformation to schwertmannite based on FT-IR results. This phase transformation resulted in rapid aggregation in all water chemistries tested, whereas other salt species affected the aggregation primarily by ion adsorption and charge screening. Presence of increasing concentrations of the organic acids significantly shifted the pH IEP of FNPs (7.0 ± 0.2) to lower pH (< 4.0) due to adsorption of organics on FNPs surfaces making them negatively charged. The adsorption of HA/FA inhibited FNP aggregation significantly while CH 3 COONa did not, due to different effects on steric and/or electrosteric interactions among FNPs by organics with varied pK a values and molecular weights. After accounting for the important effects of pH, electrolytes, and organics in modifying FNPs' surface charge, DLVO calculations agreed well with measured critical coagulation concentrations (CCC) values of FNPs at both pH 5.0 ± 0.1 and 7.0 ± 0.1 in the presence of NaCl. This study will hence be useful to better predict and control the fate and transport of FNPs in the presence of electrolytes and organics with different molecular weights, as well as the fate of the associated contaminants in natural and engineered systems., (Copyright © 2019. Published by Elsevier Inc.)

Seawater reverse osmosis (SWRO) is a commonly used desalination technique owing to its lesser environmental and economic impacts as compared to thermal desalination techniques. Antiscalants are used in SWRO to reduce membrane scaling caused by the supersaturation of salts present in feed water. However, to remain effective in reducing membrane scaling, antiscalants should be highly stable and resistant to biological degradation by seawater microorganisms. In this research, several bacteria from Qatar's seawater were isolated and screened for their ability to use antiscalants as a carbon and energy source. The biodiversity of antiscalant degrading seawater bacteria was demonstrated through combining the techniques of MALDI-TOF MS and principle component analysis. It was found that the bacteria isolated from Qatar's seawater such as H. aquamarina, H. elongata, P. fragi, P. stutzeri and others can degrade antiscalants and use them as a carbon and energy source. It was observed that the growth rates varied based on the type of antiscalant and the bacteria used. Among the tested strains, H. aquamarina, which is also known for its potential to cause biofouling, demonstrated the highest growth rates in antiscalants media. Thus, it was concluded that there is wide variety of bacteria in Qatar's seawater that can biodegrade the antiscalants; reducing their efficiency to combat membrane scaling. Since, these antiscalants will be used as a source of carbon and energy, microbial growth will increase resulting in enhanced membrane biofouling in SWRO., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Improving the colloidal stability of magnetite nanoparticles (MNPs) is essential for their successful applications. In this study, the surface zeta potential and particle size evolutions of citric acid coated magnetite nanoparticles (CA-MNPs) were measured under varied aqueous conditions using dynamic light scattering (DLS). The effects of pH (5.0-9.0), ionic strength (IS), cations (Na + and Ca 2+ ), anions (phosphate, sulfate, and chloride) and humic acid on the aggregation behaviors of CA-MNPs were explored. Compared with bare MNPs, the stability of CA-MNPs were greatly improved over the typical pH range of natural aquatic environments (pH = 5.0-9.0), as the coated CA-MNPs were highly negatively charged over the pH range due to the low pK a1 value (3.13) of citrate acid. CA-MNPs were more stable in the presence of monovalent cation (Na + ) compared with divalent cation (Ca 2+ ), as Ca 2+ could neutralize the surface charge of MNPs more significantly than Na + . In the presence of anions, the surface charges of CA-MNPs became more negative, and the stability of CA-MNPs followed the order: in phosphate > sulfate > chloride. The observed aggregation trend could be explained by the differences in the valences of the anions and their adsorption behaviors onto CA-MNPs, which altered the surface charges of CA-MNPs. The measured critical coagulation concentrations (CCC) values of CA-MNPs in these electrolyte solutions agreed well with Derjaguin-Landau-Verwey-Overbeek (DLVO) calculations. With the addition of Humic acid (HA), the aggregation of CA-MNPs was inhibited in all electrolyte solutions even with the critical coagulation concentrations. This is due to the adsorption of HA onto CA-MNPs, which enhanced the electrostatic and steric repulsive forces between CA-MNPs. Considering the good stability of CA-MNPs in solutions with varied pH and electrolyte compositions, as well as with the easy synthesis of CA-MNPs and their non-toxicity, this study suggested CA coating as a good strategy to increase the stability of MNPs., (Copyright © 2017 Elsevier Inc. All rights reserved.)

Silica aerogel, with mesoporous structure and high hydrophobicity, is a promising adsorbent for oil spill clean-up. To make it economic and environmental-friendly, hydrocarbon desorption and silica aerogel regeneration were investigated. After hydrocarbon desorption at 80°C, silica aerogel maintained its hydrophobicity. After toluene, petrol, and diesel desorption, shrinkage of mesopores (from 19.9 to 16.8, 13.5, and 13.4nm) of silica aerogels occurred, causing decreased adsorption capacities (from 12.4, 11.2, and 13.6 to 12.0, 6.5, and 2.3g/g). Low surface tension of petrol caused high stress on mesopores during its desorption, resulting in significant pore shrinkage. For diesel, its incomplete desorption and oxidation further hindered the regeneration. Therefore, diesel desorption was also conducted at 200°C. Severe diesel oxidation occurred under aerobic condition and destroyed the mesopores. Under anaerobic condition, no diesel oxidation occurred and the decreases in pore size (to 13.2nm) and adsorption efficiency (to 10.0g/g) of regenerated silica aerogels were much less, compared with under aerobic condition. This study provided new insights on silica aerogel regeneration for oil spill clean-up., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

The fluorine content of coal has been well documented, while such data of coal spoil are limited. In the present paper, fluorine in coal spoils and its releasing behavior were studied via leaching and combustion tests, as well as field investigation. Fluoride pollution in groundwater and soil occurred in the air depositing areas of coal spoils. The average content of fluorine in coal spoils was 525 mg/kg with the highest value of 1885 mg/kg. The only XRD detectable inorganic fluorine phase was fluorphlogopite. The absence of major fluorine bearing minerals in coal spoils suggested that bulk fluorine, rather than trace phases, resided in the mineral matrix. The major extracted species were water soluble fluorine and exchangeable fluorine in the coal spoils. Batch leaching tests illustrated that the leachable fluoride in coal spoils was widely distributed, ranging from 2.0 to 108.4 mg/kg. Column leaching tests showed a clear pH-dependent leaching behavior of fluorine: lower pH situation led to fluorine release from the mineral matrix; the loosely bound or easily exchangeable fluorine was also flushed out of the column. The higher ion strength or alkaline bicarbonate/carbonate rich leaching solution tended to free more fluorine into the acidic aqueous solution. The leachable fluorine in coal spoils was estimated as ca. 6%, based on the results of leaching tests. Also, our research found that over 90% of fluorine in coal spoils could be released into the atmosphere as a result of spontaneous combustion, accounting for over 40% of the total atmospheric fluorine emissions in northern China. Our investigation suggests that it is urgent to conduct comprehensive studies to assist the management and control of fluorine pollution at coal spoil banks., (Copyright © 2015. Published by Elsevier B.V.)

Volatile Organic Compounds (VOCs) exposure can induce a range of adverse human health effects. To date, however, personal VOCs exposure and residential indoor and outdoor VOCs levels have not been well characterized in the mainland of China, less is known about health risk of personal exposure to VOCs. In this study, personal exposures for 12 participants as well as residential indoor/outdoor, workplace and in vehicle VOCs concentrations were measured simultaneously in Tianjin, China. All VOCs samples were collected using passive samplers for 5 days and were analyzed using Thermal Desorption GC-MS method. U.S. Environmental Protect Agency's Inhalation Unit Risks were used to calculate the inhalation cancer health risk. To assess uncertainty of health risk estimate, Monte Carlo simulation and sensitivity analysis were implemented. Personal exposures were greater than residential indoor exposures as expected with the exception of carbon tetrachloride. Exposure assessment showed modeled and measured concentrations are statistically linearly correlated for all VOCs (P<0.01) except chloroform, confirming that estimated personal exposure using time-weighted model can provide reasonable estimate of personal inhalation exposure to VOCs. Indoor smoking and recent renovation were identified as two major factors influencing personal exposure based on the time-activity pattern and factor analysis. According to the cancer risk analysis of personal exposure, benzene, chloroform, carbon tetrachloride and 1,3-butadiene had median upper-bound lifetime cancer risks that exceeded the U.S. EPA benchmark of 1 per one million, and benzene presented the highest median risks at about 22 per one million population. The median cumulative cancer risk of personal exposure to 5 VOCs was approximately 44 per million, followed by indoor exposure (37 per million) and in vehicle exposure (36 per million). Sensitivity analysis suggested that improving the accuracy of exposure measurement in further research would advance the health risk assessment., (Copyright © 2010 Elsevier B.V. All rights reserved.)

Nineteen road dust samples were collected during 2005 in different parts of the urban area of Anshan, Liaoning Province, China, and 11 polycyclic aromatic hydrocarbons (PAHs) species were quantitatively analyzed using GC-MS. The results indicated that the total average concentration of PAHs over the investigated sites ranged from 48.73 to 638.26 microg/g, with a mean value of 144.25 microg/g, higher than the concentrations measured in previous studies. PAHs concentrations were higher with high molecular weight homologues (4-6 rings PAHs), accounting for 83.24-96.98%, showing combustion of petroleum fuels was a potential source. Organic carbon in road dust was considered one of the important factors that influenced the concentrations of PAHs in this study, and it was found that concentrations of total PAHs were correlated with those of organic carbon in road dust. The results of diagnostic ratios analysis showed traffic emission (gasoline or diesel) was one of the most important sources of road dust PAHs. Principal component analysis (PCA) indicated that the major sources of road dust PAHs might be emission from traffic, steel industry, cooking and coal combustion.

In China, traffic policemen have to stand for several hours a day at the road intersections with high vehicle flows. To assess their exposure to airborne carcinogenic polycyclic aromatic hydrocarbons (PAHs) during their working time, a preliminary study was conducted to measure the personal exposure level to PAHs. And a probabilistic incremental lifetime cancer risk (ILCR) model together with the benzo[a]pyrene (BaP) toxic equivalents (BaP(eq)) method was used to conduct health risk assessment. Personal exposure monitors (PEM) were carried by traffic policemen to collect PM10 samples during their daily work in Tianjin, China. Meanwhile, PM100 samples were collected at the roadsides and on campus of Nankai University as comparison. PAHs species were quantitatively analyzed by GC/MS. Experimental results showed that the concentrations of total PAHs, BaP and BaP(eq) were much higher at the road intersections (867.5, 26.2, 82.4 ng m(-3)), where the traffic policemen stand during their work time, than those at the roadsides (46.6, 1.5, 5.7 ng m(-3)), and on campus (19.5, 0.7, 2.4 ng m(-3)). According to the risk assessment results, the occupational risk falls within the range from 10(-6) to 10(-3). On the basis of sensitivity analysis results, further research should be directed to give better characterization of the yearly concentration distribution of PAHs and the cancer slope factor (CSF) of BaP in order to improve the accuracy of the health risk assessment.