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Enzymatic probe sonication for quick extraction of total bisphenols from animal-derived foods: Applicability to occurrence and exposure assessment
2022
Xiao, Zhiming | Wang, Shi | Suo, Decheng | Wang, Ruiguo | Huang, Yuan | Su, Xiaoou
A high demand exists in bisphenols (BPs) screening studies for quick, reliable and straightforward analytical methods that generate data faster and simultaneously. Herein, we describe a combination of enzymatic probe sonication (EPS) and ultra-performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) for quick extraction and simultaneous quantification of eight important BPs in animal-derived foods. Results obtained demonstrated that the ultrasonic probe power could not only enhance the enzymatic hydrolysis efficiency, but also accelerate the liquid-liquid extraction procedure. Under optimized EPS parameters, one sample could be exhaustively extracted within 120 s, as compared with 12 h needed for the conventional enzymatic extraction which is more suitable for high-throughput analysis. The method was successfully applied to analyze residual BPs in animal-derived foods collected from Beijing, China. Widespread occurrence of BPA, BPS, BPF, BPAF, BPP, and BPB were found, with detection frequencies of 65.2%, 42.4%, 33.7%, 29.4%, 28.3%, and 27.2%, respectively. The highest total concentration levels of BPs (sum of the eight BPs analyzed, ΣBPs) were found in chicken liver (mean 12.2 μg/kg), followed by swine liver (6.37 μg/kg), bovine muscle (3.24 μg/kg), egg (2.03 μg/kg), sheep muscle (2.03 μg/kg), chicken muscle (1.45 μg/kg), swine muscle (1.42 μg/kg), and milk (1.17 μg/kg). The estimated daily intake (EDI) of BPs, based on the mean and 95th percentile concentrations and daily food consumptions, was estimated to be 5.687 ng/kg bw/d and 22.71 ng/kg bw/d, respectively. The human health risk assessment in this work suggests that currently BPs do not pose significant risks to the consumers because the hazard index (HI) was <1.
Показать больше [+] Меньше [-]Fabrication of mesoporous nanocomposite of graphene oxide with magnesium ferrite for efficient sequestration of Ni (II) and Pb (II) ions: Adsorption, thermodynamic and kinetic studies
2019
Nawanīta Kaura, | Manpreet Kaur, | Singh, Dhanwinder
Mesoporous nanocomposite of MgFe₂O₄ nanoparticles (NPs) and graphene oxide (GO) was synthesized using facile sonication method. Its potential was tested for the removal of Ni (II) and Pb (II) ions from water. The 2:1 w/w ratio of MgFe₂O₄:GO was optimum for the maximum removal of metal ions. Nanocomposite was characterized employing XRD, FT-IR, VSM, SEM-EDX, XPS, TEM and BET analyses. It possessed higher surface area (63.0 m² g⁻¹) than pristine NPs. Batch experiments were performed to study the effect of process parameters viz. pH, dose, contact time, initial metal ion concentration, co-existing ions and temperature. Statistical parameters were also determined. Langmuir, Temkin and Freundlich models were followed in perfect way. Langmuir model showed the monolayer adsorption of metal ions onto the homogeneous surface of nanocomposite with maximum adsorption capacity of 100.0 mg g⁻¹ and 143.0 mg g⁻¹ for Ni (II) and Pb (II) ions respectively, which was higher than the same for MgFe₂O₄ NPs and GO. Kinetic studies demonstrated that the pseudo-second order model well described the adsorption process. The ΔS° and ΔG° values revealed spontaneous nature of adsorption process. Positive ΔH° values using MgFe₂O₄ NPs and nanocomposite indicated endothermic removal; whereas using GO the removal was exothermic. The observed trend for coexisting ions correlated with hydrated ion radii. Efficiency of the adsorbents was also tested for realistic nickel electroplating industrial effluent. Apart from the higher adsorption potential of nanofabricated composite, its magnetic properties are advantageous in utilizing metal loaded nanocomposite for adsorption-desorption cycles for reuse.
Показать больше [+] Меньше [-]Magnetic metal-organic frameworks nanocomposites for negligible-depletion solid-phase extraction of freely dissolved polyaromatic hydrocarbons
2019
Li, Yingjie | Zhou, Xiaoxia | Dong, Lijie | Lai, Yujian | Li, Shasha | Liu, Rui | Liu, Jingfu
The bioavailability of a pollutant is usually evaluated based on its freely dissolved concentration (Cfree), which can be measured by negligible-depletion equilibrium extraction that is commonly suffered from long equilibration time. Herein, metal-organic framework (MOF) composites (Fe3O4@MIL-101), consists of a magnetic Fe3O4 core and a MIL-101 (Cr) MOF shell, is developed as sorbents for negligible-depletion magnetic solid-phase extraction (nd-MSPE) of freely dissolved polyaromatic hydrocarbons (PAHs) in environmental waters. The freely dissolved PAHs in 1000 mL water samples are extracted with 1.5 mg MOF composites, and desorbed with 0.9 mL of acetonitrile under sonication for 5 min. The MOF composites exclude the extraction of dissolved organic matter (DOM) and DOM-associated PAHs by size exclusion. Additionally, the combined interactions (hydrophobic, π-π and π-complexation) between PAHs and composites markedly reduced the extraction equilibration time to < 60 min for all the studied PAHs with logKOW up to 5.74. Moreover, the porous coordination polymers property of the MOFs makes the proposed nd-MSPE based on the partitioning of PAHs and thus excludes the competitive adsorption of coexisting substances. The developed nd-MSPE approach provides low detection limits (0.08–0.82 ng L−1), wide linear range (1–1000 ng L−1) and high precision (relative standard deviations (RSDs) (3.3–4.8%) in determining Cfree of PAHs. The measured Cfree of PAHs in environmental waters are in good agreement with that of verified method. Given the large diversity in structure and pore size of MOFs, various magnetic MOFs can be fabricated for task-specific nd-MSPE of analytes, presenting a prospective strategy for high-efficiency measuring Cfree of contaminants in environments.
Показать больше [+] Меньше [-]Enhanced removal of per- and polyfluoroalkyl substances in complex matrices by polyDADMAC-coated regenerable granular activated carbon
2022
Ramos, Pia | Singh Kalra, Shashank | Johnson, Nicholas W. | Khor, Chia Miang | Borthakur, Annesh | Cranmer, Brian | Dooley, Gregory | Mohanty, Sanjay K. | Jassby, David | Blotevogel, Jens | Mahendra, Shaily
Granular activated carbon (GAC) has been used to remove per- and polyfluoroalkyl substances (PFASs) from industrial or AFFF-impacted waters, but its effectiveness can be low because adsorption of short-chained PFASs is ineffective and its sites are exhausted rapidly by co-contaminants. To increase adsorption of anionic PFASs on GAC by electrostatic attractions, we modified GAC's surface with the cationic polymer poly diallyldimethylammonium chloride (polyDADMAC) and tested its capacity in complex water matrices containing dissolved salts and humic acid. Amending with concentrations of polyDADMAC as low as 0.00025% enhanced GAC's adsorption capacity for PFASs, even in the presence of competing ions. This suggests that electrostatic interactions with polyDADMAC's quaternary ammonium functional groups helped bind organic and inorganic ions as well as the headgroup of short-chain PFASs, allowing more overall PFAS removal by GAC. Evaluating the effect of polymer dose is important because excessive addition can block pores and reduce overall PFAS removal rather than increase it. To decrease the waste associated with this adsorption strategy by making the adsorbent viable for more than one saturation cycle, a regeneration method is proposed which uses low-power ultrasound to enhance the desorption of PFASs from the polyDADMAC-GAC with minimum disruption to the adsorbent's structure. Re-modification with the polymer after sonication resulted in a negligible decrease in the sorbent's capacity over four saturation rounds. These results support consideration of polyDADMAC-modified GAC as an effective regenerable adsorbent for ex-situ concentration step of both short and long-chain PFASs from real waters with high concentrations of competing ions and low PFAS loads.
Показать больше [+] Меньше [-]Remediation of contaminated sediments containing both organic and inorganic chemicals using ultrasound and ozone nanobubbles
2021
Most river sediments are contaminated with organic and inorganic pollutants and cause significant environmental damage and health risks. This research is evaluated an in-situ sediment remediation method using ultrasound and ozone nanobubbles to remove organic and inorganic chemicals in contaminated sediments. Contaminated sediment is prepared by mixing synthetic fine sediment with an organic (p-terphenyl) and an inorganic chemical (chromium). The prepared contaminated sediment is treated with ultrasound and ozone nanobubbles under different operating conditions. For the samples with the maximum initial concentration of 4211 mg/kg Cr and 1875 mg/kg p-terphenyl, average removal efficiencies are 71% and 60%, respectively, with 240 min of sonication with 2-min pulses, whereas 97.5% and 91.5% removal efficiencies are obtained for the same, respectively, as a single contaminant in the sediment. For the same maximum concentrations, the highest removal of p-terphenyl is 82.7% with 127.2 J/ml high energy density, and for Cr, it is 77.1% using the highest number of the treatment cycle and ozone usage with 78.75/ml energy density. The Cr highest removal efficiency of 87.2% is recorded with the reduced initial concentration of 1227 mg/kg with the highest treatment cycles. The Cr removal efficiency depends on the availability of oxidizing agents and the number of washing cycles of sediments, whereas P-terphenyl degradation is most likely influenced by the combined effects of oxidation and ultrasound-assisted pyrolysis and combustion of organics.
Показать больше [+] Меньше [-]Prenatal exposure levels of polybrominated diphenyl ethers in mother-infant pairs and their transplacental transfer characteristics in Uganda (East Africa)
2020
Matovu, Henry | Ssebugere, Patrick | Sillanpää, Mika
Polybrominated diphenyl ethers (PBDEs) are ubiquitous environmental pollutants with adverse effects on the foetus and infants. This study aimed at assessing in utero exposure levels and transplacental transfer (TPT) characteristics of BDE congeners in primiparous mothers from Kampala, the capital city of Uganda. Paired human samples (30 placenta and 30 cord blood samples) were collected between April and June 2018; and analysed for a suite of 24 tri-to deca-BDE congeners. Extraction was carried out using liquid-liquid extraction and sonication for cord blood and placenta samples, respectively. Clean-up was done on a solid phase (SPE) column and analysis was performed using gas chromatography/mass spectrometry (GC/MS). Total (∑) PBDEs were 0.25–30.9 ng/g lipid weight (lw) (median; 7.11 ng/g lw) in placental tissues and 1.65–34.5 ng/g lw (median; 11.9 ng/g lw) in cord blood serum, with a mean difference of 1.26 ng/g lw between the compartments. Statistical analysis showed no significant difference between the levels of PBDEs in cord blood and placenta samples (Wilcoxon signed rank test, p = 0.665), possibly because foetus and neonates have poorly developed systems to metabolise the pollutants from the mothers. BDE-209 was the dominant congener in both matrices (contributed 40.5% and 51.2% to ∑PBDEs in placenta and cord blood, respectively), suggesting recent and on-going maternal exposure to deca-BDE formulation. Non-significant associations were observed between ∑PBDEs in maternal placenta and maternal age, household income, pre-pregnancy body mass index (BMI), and beef/fish consumption. This suggested on-going exposure to PBDEs through multiple sources such as dust from indoor/outdoor environments and, ingestion of other foods. Based on absolute concentrations, the extent of transplacental transport was greater for higher congeners (BDE-209, -206 and −207) than for lower ones (such as BDE-47), suggesting alternative TPT mechanisms besides passive diffusion. More studies with bigger sample sizes are required to confirm these findings.
Показать больше [+] Меньше [-]Synthesis and performance evaluation of plastic waste aerogel as sustainable and reusable oil absorbent
2021
Pawar, Atul A. | Kim, Ayoung | Kim, Hern
Direct utilization of waste polyethylene terephthalate (PET) from the environment to form highly porous aerogel technology for oil absorption is an attractive approach from the view point of green chemistry. However, the oil absorption reaction is limited by low oil absorption capacity and less stability. For now, silica aerogel are used to solve these problem. Our goal is to substitute to these silica aerogel with PET aerogel technology. Herein, we have prepared an environmental waste PET based aerogel with 1.0:0.5 wt% PET, polyvinyl alcohol (PVA), and glutaraldehyde (GA) 0.2% v/v were dispersed in 10 mL DI water, followed by homogenization (30 min), sonication (10 min), and ageing (2 h) at 70 °C. To escape macroscopic cracking, cooling (8 h) at 4 °C was followed by freezing (6 h), freeze drying at −80 °C, and 5 mTorr for 18 h. The hybrid PET aerogel displays excellent performance towards oil absorption. Notably it showed high absorption capacity towards the different oils about 21–40 times its own weight, depending on the viscosity and density of the oil and solvents within 15–35 s, 25 °C, and 2 × 2 cm aerogel size. In addition, the aerogel shows there is no change in structure after several recycles due to high mechanical strength. Furthermore, because of the PET aerogel's high porosity (99.74%) and low density (0.0311 g/cm³), close bonding between PET-PVA occurs. Therefore, aerogel shows hydrophobic nature, good mechanical strength, high thermal stability, arrangement of the interconnected fibrillar pore network offers a high surface to volume ratio, low surface energy, high surface roughness, and more reusability. All these parameters are responsible for high oil absorption.
Показать больше [+] Меньше [-]Methodology to examine polycyclic aromatic hydrocarbons (PAHs) nitrated PAHs and oxygenated PAHs in sediments of the Paraguaçu River (Bahia, Brazil)
2018
Conventional methods for determination of polycyclic aromatic compounds (PACs) in sediments usually require large sample sizes (grams) and solvent volumes (at least 100 mL) through the employment of Soxhlet extraction, which is both time (hours) and energy consuming, among other disadvantages. We developed a new analytical protocol for the determination of PACs in sediments using microextraction, which requires small sample masses (25 mg), 500 μL of acetonitrile-dichloromethane mix and sonication for 23 min, followed by GC–MS analysis. The method was validated using the certified reference material SRM 1941b – NIST organic marine sediment, as well as internal deuterated standards. Seventeen PAHs, seven nitro-PAHs and one quinone were detected and quantified. The mean concentrations were 90.4 ng g−1 for PAHs, 179.2 ng g−1 for nitro-PAHs and 822.5 ng g−1 for quinones. The proposed method showed good sensitivity, linearity, precision and accuracy for the determination of PAC in sediments samples.
Показать больше [+] Меньше [-]Microplastics as vectors of metals contamination in Mediterranean Sea
2022
Squadrone, Stefania | Pederiva, Sabina | Bezzo, Tabata | Sartor, Rocco Mussat | Battuello, Marco | Nurra, Nicola | Griglione, Alessandra | Brizio, Paola | Abete, Maria Cesarina
Microplastics are contaminants of great concern all over the world. Microplastics constitute pollutants themselves; moreover, other contaminants such as metals are easily absorbed on their plastic surface, becoming bioavailable to marine biota such as zooplankton.We collected marine zooplankton from Mediterranean Sea to investigate trace elements associated with microplastics. Samples were subjected to visual sorting by a stereomicroscope, collected with sterile tweezers, pooled and subjected to sonication, filtration, and drying before being subjected to acid extraction. An ICP-MS was utilized for multi-elemental determination.Aluminum, iron, chromium, zinc, nickel, molybdenum, manganese, lead cobalt, and copper were found at concentrations of mg/kg while arsenic, vanadium, rubidium, and cadmium at level of μg kg⁻¹. Other elements such as silver, beryllium, bismuth, selenium, tin, and thallium were under the limit of quantitation. Lower levels of iron and manganese in samples from Italy were found in comparison to England and Brazil, while aluminum, copper, and zinc registered comparable values. The presence of metals in marine waters is strictly related to sediment lithology and anthropogenic inputs, but plastic plays a key role as vectors for metal ions in the marine system, being able to concentrate metals several order of magnitude higher than in surrounding waters and exerting potential toxicity for living beings after chronic exposure.
Показать больше [+] Меньше [-]Trihexyl tetradecyl phosphonium bromide as an effective catalyst/extractant in ultrasound-assisted extractive/oxidative desulfurization
2022
Desai, Komal | Dharaskar, Swapnil | Pandya, Jalaja | Shinde, Satyam | Gupta, Thummalapalli
Phosphonium-based ionic liquid (PIL) has been used as a catalyst and extractant. Here, the PIL, trihexyl tetradecyl phosphonium bromide ([THTDP]Br) was utilized for the S-removal of model oil (MO) and acted as the reaction-induced self-separation catalyst. The influence of oxidant to sulfur molar ratio (n(O/S)), mass ratio of model oil to ionic liquid (m(MO/IL)), sonication time, and temperature was observed to investigate the optimal conditions for the ultrasound-assisted extractive/oxidative desulfurization (UEODS) catalyzed by [THTDP]Br. A kinetic study was performed, and the reaction rate constant and half-life were calculated as the oxidation reaction was following pseudo-first-order reaction kinetics. Moreover, the oxidation reactivity and selectivity of various sulfur substrates were in the following order: DBT > BT > TH > 3-MT. The DBT removal with various initial S-content was observed to be constant, which makes it feasible for practical application. The interaction energy between [THTDP]Br and S-compounds was examined using Density Functional Theory. The sulfur removal of base oil (BO) was also examined using various desulfurization systems at DBT optimized conditions. The highest desulfurization efficiency of BO was obtained during the UEODS process, which made it industrially feasible. [THTDP]Br was regenerated and recycled six times with a slight variation in efficiency.
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