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Performance comparison of silicone and low-density polyethylene as passive samplers in a global monitoring network for aquatic organic contaminants
2022
Sobotka, Jaromír | Smedes, Foppe | Vrana, Branislav
Contamination with hydrophobic organic compounds (HOCs) such as persistent organic pollutants negatively affects global water quality. Accurate and globally comparable monitoring data are required to understand better the HOCs distribution and environmental fate. We present the first results of a proof-of-concept global monitoring campaign, the Aquatic Global Passive Sampling initiative (AQUA-GAPS), performed between 2016 and 2020, for assessing trends of freely dissolved HOC concentrations in global surface waters. One of the pilot campaign aims was to compare performance characteristics of silicone (SSP) and low-density polyethylene (PE) sheets co-deployed in parallel under identical conditions, i.e. at the same site, using the same deployment design, and for an equal period. Individual exposures lasted between 36 and 400 days, and samples were collected from 22 freshwater and 40 marine locations. The sampler inter-comparability is based on a rationale of common underlying principles, i.e. HOC diffusion through a water boundary layer (WBL) and absorption by the polymer. In the integrative uptake phase, equal surface-specific uptake in both samplers was observed for HOCs with a molecular volume less than 300 ų. For those HOCs, transport in the WBL controls the uptake as mass transfer in the polymer is over 20-times faster. In such a case, sampled HOC mass can be converted into aqueous concentrations using available models derived for WBL-controlled sampling using performance reference compounds. In contrast, for larger molecules, surface-specific uptake to PE was lower than to SSP. Diffusion in PE is slower than in SSP, and it is likely that for large molecules, diffusion in PE limits the transport from water to the sampler, complicating the interpretation. Although both samplers provided mostly well comparable results, we recommend, based on simpler practical handling, simpler data interpretation, and better availability of reliable polymer-water partition coefficients, silicone-based samplers for future operation in the worldwide monitoring programme.
显示更多 [+] 显示较少 [-]Adsorptive removal of propranolol under fixed-bed column using magnetic tyre char: Effects of wastewater effluent organic matter and ball milling
2022
Feizi, Farzaneh | Sarmah, Ajit K. | Rangsivek, Ropru | Gobindlal, Kapish
We investigated the competitive effects of different fractions of wastewater treatment plant effluent organic matter (EfOM) on adsorption of an organic micro pollutant (OMP), propranolol (PRO), in a fixed bed column packed with magnetic tyre char (MTC). The results showed that the presence of EfOM inhibited PRO adsorption in wastewater leading to decreased PRO adsorption capacity from 5.86 to 2.03 mg/g due to competitive effects and pore blockage by smaller EfOM fractions. Characterization of EfOM using size exclusion chromatography (LC-OCD) showed that the principal factor controlling EfOM adsorption was pore size distribution. Low molecular weight neutrals had the highest adsorption onto MTC while humic substances were the least interfering fraction. Effect of important parameters such as contact time, linear velocity and bed height/diameter ratio on MTC performance was studied in large-lab scale columns. Linear velocity and contact time were found to be effective in increasing adsorption capacity of PRO on MTC and delaying breakthrough time. Increase in linear velocity from 0.64 cm/min to 1.29 cm/min increased mass transfer and dispersion, resulting in considerable rise of adsorbed amount (5.86 mg/g to 22.58 mg/g) and increase in breakthrough time (15.8–62.7 h). Efficiency of non-equilibrium Hydrus model considering dispersion and mass transfer mechanism was demonstrated for real wastewater and scale up purposes. Ball milling for degradation of adsorbed PRO and regeneration of MTC resulted in 79% degradation of PRO was achieved after 5 h milling (550 rpm), while the addition of quartz sand increased the efficiency to 92%.
显示更多 [+] 显示较少 [-]Volatility of Springtime ambient organic aerosol derived with thermodenuder aerosol mass spectrometry in Seoul, Korea
2022
Kang, Hyun Gu | Kim, Youngjin | Collier, Sonya | Zhang, Qi | Kim, Hwajin
The volatilities of ambient organic aerosol (OA) components are important to forecasting OA formation with models. However, providing the OA volatility distribution inputs for models is challenging, and models often rely on measurements from chamber experiments. We measured the volatility of submicron ambient OA in Seoul during May/June of 2019 by connecting a thermodenuder to an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS). We calculated a volatility basis set (VBS) of the organic aerosol with a thermodenuder mass transfer model and data from the thermodenuder set to various temperatures (30–200 °C). We found a large discrepancy between the measured ambient VBS and a reference VBS used in air quality models, with the ambient organics being less volatile. The results suggest that a modeling study that tries to account for this discrepancy may be needed to identify the impact it has on modeling outcomes. Chamber experiments aiming to determine VBSs for specific chemical systems should address limitations caused by wall losses and incomplete modeling parameters.
显示更多 [+] 显示较少 [-]Elucidating the co-transport of bisphenol A with polyethylene terephthalate (PET) nanoplastics: A theoretical study of the adsorption mechanism
2021
Cortés-Arriagada, Diego
Polyethylene terephthalate (PET) is a possible key component of nanoplastics in water environments, which can migrate pollutants through co-transport. In this regard, the co-transport of endocrine disruptors (such as bisphenol A, BPA) by nanoplastics is of emergent concern because of its cytotoxicity/bioaccumulation effects in aquatic organisms. In this work, a computational study is performed to reveal the BPA adsorption mechanism onto PET nanoplastics (nanoPET). It is found that the outer surface of nanoPET has a nucleophilic nature, allowing to increase the mass transfer and intraparticle diffusion into the nanoplastic to form stable complexes by inner and outer surface adsorption. The maximum adsorption energy is similar (even higher) in magnitude with respect to nanostructured adsorbents such as graphene, carbon nanotubes, activated carbon, and inorganic surfaces, indicating the worrying adsorption properties of nanoPET. The adsorption mechanism is driven by the interplay of dispersion (38–49%) and electrostatics effects (43–50%); specifically, dispersion effects dominate the inner surface adsorption, while electrostatics energies dominate the outer surface adsorption. It is also determined that π–π stacking is not a reliable interaction mechanism for aromatics on nanoPET. The formed complexes are also highly soluble, and water molecules behave as non-competitive factors, establishing the high risk of nanoPET to adsorb and migrate pollutants in water ecosystems. Furthermore, the adsorption performance is decreased (but not inhibited) at high ionic strength in salt-containing waters. Finally, these results give relevant information for environmental risk assessment, such as quantitative data and interaction mechanisms for non-biodegradable nanoplastics that establish strong interactions with pollutants in water.
显示更多 [+] 显示较少 [-]Synthesis of nano-magnetic MnFe2O4 to remove Cr(III) and Cr(VI) from aqueous solution: A comprehensive study
2020
Eyvazi, Behzad | Jamshidi-Zanjani, Ahmad | Darban, Ahmad Khodadadi
The co-precipitation method was used to synthesize nano-magnetic adsorbent MnFe₂O₄ (nMFO), characterized through XRD, SEM, EDS, and BET techniques. The synthesized nMFO was used for hexavalent and trivalent chromium ions elimination from the aqueous phase. The optimum pH for the adsorption of Cr (VI) and Cr (III) was determined as 2 and 5, respectively. The chromium ions adsorption behavior was well interpreted through the pseudo-second order kinetics model. Furthermore, isotherm studies were conducted, and the obtained results indicated that Langmuir isotherm model could well justify the chromium ions adsorption process. Quick removal (less than 10 min) of both chromium ions and high removal efficiency were occurred using nMFO. The utmost adsorption capacity of trivalent and hexavalent chromium ions were determined as 39.6 and 34.84 mg g⁻¹, respectively. Thermodynamic studies on chromium adsorption revealed positive value for ΔH and negative value for ΔG, representing that chromium ions adsorption was an endothermic and spontaneous process. The multilinearity in the graphs of chromium ions adsorption was observed using intra-particle diffusion model. In this regard, the external mass transfer of chromium ions on synthesized nanoparticles was the important and controlling step in the adsorption process.
显示更多 [+] 显示较少 [-]Influence of some physicochemical parameters on the passive sampling of copper (II) from aqueous medium using a polymer inclusion membrane device
2020
González-Albarrán, René | de Gyves, Josefina | Rodríguez de San Miguel, Eduardo
Recently polymer inclusion membranes (PIMs) have been proposed as materials for passive sampling, nonetheless a theoretical base to describe the mass transfer process through those materials, under such conditions of monitoring, has not been elucidated. Under the assumption that: (i) the transport of the metal ion occurs at steady state conditions, (ii) the concentration gradients are linear, and (iii) the kinetics of the chemical reactions in the extraction process on the membrane are elemental; an equation for the passive sampling of copper (II) using a PIM system containing Kelex-100 as carrier is derived. The prediction capacity of this sampler under different conditions of temperature, metal concentration, flow velocity, ionic strength and pH is analyzed as well. Among the dependencies of the PIM on the physicochemical conditions, effects of concentration, temperature and flow velocity tend to increment copper (II) flux across the membrane, being the parameter temperature the one with the most pronounced effect at T ≥ 30 °C. Ionic strength had no great effect on passive sampler response, however the sampler is dependent on the acidity of the medium. The comparable metal ion concentrations estimated from the PIM sampler to those obtained by direct measurements of the sampling medium suggest that PIMs can be robust materials when used as passive sampler devices.
显示更多 [+] 显示较少 [-]Comparative analysis on the sorption kinetics and isotherms of fipronil on nondegradable and biodegradable microplastics
2019
Gong, Wenwen | Jiang, Mengyun | Han, Ping | Liang, Gang | Zhang, Tingting | Liu, Guannan
Biodegradable plastics have been introduced and widely used as a promising alternative to traditional nondegradable plastics. However, the differences in sorption behavior of pesticides on nondegradable and biodegradable microplastics has been insufficiently studied. Here, four types of nondegradable [polyethylene (PE), polystyrene (PS), polyvinyl chloride (PVC), polypropylene (PP)] and two types of biodegradable [polylactic acid (PLA), polybutylene succinate (PBS)] microplastics were selected to investigate the sorption mechanism of fipronil based on their sorption kinetics and isotherms. The results indicated that the sorption rates of PLA and PBS were much higher than those of PE, PP, PVC and PS and that the sorption capacities of fipronil on microplastics followed the order of PBS > PLA > PP > PE > PS > PVC. The sorption kinetics followed a pseudo-second-order kinetics model (R² = 0.953–0.998) for all tested microplastics. External mass transport and intraparticle diffusion were the main rate controlling steps of the sorption of fipronil on microplastics. Furthermore, isotherm results indicated that a Langmuir model provided the best fit for fipronil sorption on PE, PS, PVC and PP (R² = 0.997–0.999), while a Freundlich model was the most appropriate model for PLA and PBS (R² = 0.998–0.999). The presence of surface O-containing functional groups and the spatial arrangement of rubbery domains are likely to affect the sorption process. The results from this work suggest that microplastics, especially biodegradable ones, may play an important role in the fate and transport of pesticides, and their effects on soil organisms (e.g., earthworms) require further investigation.
显示更多 [+] 显示较少 [-]Mechanistic insight into the adsorption of diclofenac by MIL-100: Experiments and theoretical calculations
2019
Zhuang, Shuting | Liu, Yong | Wang, Jianlong
The development of high-efficiency adsorbents and the exploration of their adsorption mechanisms are major challenges in environmental remediation. Herein, MIL-100 was prepared, characterized, and utilized for the adsorptive removal of diclofenac sodium (DCF) from aqueous solutions. A high monolayer adsorption capacity of 773 mg g⁻¹ was recorded. The adsorption mechanism was proposed based on different contributions of two types of pore structure of MIL-100 to the adsorption of DCF from aqueous solutions according to the experimental results and theoretical calculation. During adsorption process, DCF (5.2 × 7.4 × 10.3 Å) diffused through the free area of hexagonal pores (8.6 × 8.6 Å) into the cages of MIL-100, whilst it was adsorbed by the pentagonal pores (4.8 × 5.8 Å) preferentially. Internal mass transfer resistance, which was identified as one of the dominant rate-limiting steps by the mass transfer resistance kinetic models based on the Sips model, will be derived from the diffusion process, which was affected by the size-sieving effect of the pore structure of MIL-100. The successful diffusion of DCF into the interior of MIL-100 and the stable configuration between MIL-100 and DCF accounted for the high adsorption capacity. The capture of DCF into MIL-100 also resulted in the pore size distribution variation of adsorbent, which provided vital experimental evidence for the proposed mechanism. This study may offer deeper insights into other pollutants removal by metal-organic frameworks type adsorbents.
显示更多 [+] 显示较少 [-]The phenomenological mass transfer kinetics model for Sr2+ sorption onto spheroids primary microplastics
2019
Guo, Xuan | Wang, Jianlong
In this paper, the equilibrium and mass transfer kinetics of Sr2+ sorption onto 3 types of microplastics, including polyethylene terephthalate (PET), polyethylene (PE), and polyvinyl chloride (PVC) were investigated. A novel film-pore mass transfer (FPMT) model was developed and used to study the sorption kinetics and mechanisms. This model can be used to describe the external mass transfer (EMT) and the internal mass transfer (IMT) processes and to calculate the diffusion rate. The FPMT model could successfully predict the kinetics data of Sr2+ sorption onto microplastics. The maximum value of the EMT rate achieved at the beginning of sorption was 103 μg g−1·h−1 for PET, 247 μg g−1·h−1for PE, and 854 μg g−1·h−1 for PVC, and then it decreased dramatically with time. The IMT rate was far less than the EMT rate, and decreased slowly with time. The overall sorption rate of Sr2+ onto microplastics was controlled by the external mass transfer step.
显示更多 [+] 显示较少 [-]Adsorption mechanism of As(III) on polytetrafluoroethylene particles of different size
2019
Dong, Youming | Gao, Minling | Song, Zhengguo | Qiu, Weiwen
Microplastics exhibit active environmental behavior and unique surface characteristics, and act as carriers for the migration of trivalent arsenic (As(III)) in the environment. Herein, the mechanism by which polytetrafluoroethylene (PTFE) microplastic particles adsorb As(III) is systematically determined. The larger the size of PTFE particles, the smaller the specific surface area, the higher the point of zero charge (PZC), and the more unfavorable adsorption of As(III); the highest adsorption amount can reach 1.05 mg g⁻¹. The adsorption process can be divided into three stages by the intraparticle diffusion model: external mass transfer, intraparticle diffusion, and dynamic equilibrium, of which the external mass transfer stage is the adsorption rate-limiting stage. The Langmuir isotherm model better represented the equilibrium adsorption results. The adsorption of As(III) by PTFE was an exothermic process, and because the increase in temperature broke the hydrogen bond, the amount of adsorption was decreased, which was not conducive to spontaneous adsorption. In the pH range of 3–7, as the pH value increased, the amount of As(III) adsorbed by PTFE gradually decreased, which may be related to the change in PZC for PTFE and the protonation of As(III). The H on the surface hydroxyl group of the PTFE exhibited a very large positive potential (+82.37 kcal mol⁻¹). Thus, it can attract the arsenic oxyanion, and As(III) was subsequently adsorbed on the surface of the PTFE through the hydrogen bond on the hydroxyl group. Electrostatic force and non-covalent interaction were the key mechanisms affecting the PTFE adsorption.
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