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Non-target screening of micropollutants and transformation products for assessing AOP-BAC treatment in groundwater
2022
Tisler, Selina | Tüchsen, Peter L. | Christensen, Jan H.
Standard monitoring programs give limited insight into groundwater status, especially transformation products (TPs) formed by natural processes or advanced oxidation processes (AOP), are normally underrepresented. In this study, using suspect and non-target screening, we performed a comprehensive analysis of groundwater before and after AOP by UV/H₂O₂ and consecutively installed biological activated carbon filters (BAC). By non-target screening, up to 413 compounds were detected in the groundwater, with an average 70% removal by AOP. However, a similar number of compounds were formed during the process, shown in groundwater from three waterworks. The most polar compounds were typically the most stable during the AOP. A subsequent BAC filter showed removal of 95% of the TPs, but only 46% removal of the AOP remaining precursors. The BAC removal for polar compounds was highly dependent on the acidic and basic functional groups of the molecules. 49 compounds of a wide polarity range could be identified by supercritical fluid chromatography (SFC) and liquid chromatography (LC) with high resolution mass spectrometry (HRMS); of these, 29 compounds were already present in the groundwater. To the best of our knowledge, five compounds have never been reported before in groundwater (4-chlorobenzenesulfonic acid, dibutylamine, N-phenlybenzenesulfonamide, 2-(methylthio)benzothiazole and benzothiazole-2-sulfonate). A further five rarely reported compounds are reported for the first time in Danish groundwater (2,4,6-trichlorophenol, 2,5-dichlorobenzenesulfonic acid, trifluormethansulfonic acid, pyrimidinol and benzymethylamine). Twenty of the identified compounds were formed by AOP, of which 10 have never been reported before in groundwater. All detected compounds could be related to agricultural and industrial products as well as artificial sweeteners. Whereas dechlorination was a common AOP degradation pathway for chlorophenols, the (ultra-) short chain PFAs showed no removal in our study. We prioritized 11 compounds as of concern, however, the toxicity for many compounds remains unknown, especially for the TPs.
Show more [+] Less [-]Fabrication of activated carbon supported modified with bimetallic-platin ruthenium nano sorbent for removal of azo dye from aqueous media using enhanced ultrasonic wave
2022
Herein, activated carbon supported modified with bimetallic-platin ruthenium nano sorbent (PtRu@AC) was synthesized by a thermal decomposition process and used in the removal of methylene blue (MB) from aqueous solutions. The synthesized nano sorbents were characterized by X-ray Diffraction (XRD), Transmission Electron Microscopy (TEM), and X-ray Photoelectron Spectroscopy (XPS) spectroscopic techniques. The data obtained from characterization studies showed that PtRu@AC nano sorbent was highly crystalline and in a form of PtRu alloy with a monodispersed composition. The results indicated that the maximum adsorption capacity (qemax) for the removal of MB with PtRu@AC under optimum conditions was detected to be 1.788 mmol/g (569.4 mg/g). The experimental kinetic results of the study revealed that the adsorption of methylene blue was found to be more compatible with the false second-order model compared to some tested models. Calculations for thermodynamic functions including enthalpy change (ΔHo), entropy change (ΔSo), and Gibbs free energy change (ΔGo) values were performed to get an idea about the adsorption mechanism. As a result, the synthesized PtRu@AC nano adsorbent was detected as a highly effective adsorbent material in the removal of MB from aquatic mediums.
Show more [+] Less [-]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.
Show more [+] Less [-]Carbon nanomaterials for the detection of pesticide residues in food: A review
2022
Mishra, Smriti | Mishra, Shivangi | Patel, Shiv Singh | Singh, Sheelendra Pratap | Kumar, Pradip | Khan, Mohd Akram | Awasthi, Himani | Singh, Shiv
In agricultural fields, pesticides are widely used, but their residual presence in the environment poses a threat to humans, animals, insects, and ecosystems. The overuse of pesticides for pest control, enhancement of crop yield, etc. leaves behind a significant residual amount in the environment. Various robust, reliable, and reusable methods using a wide class of composites have been developed for the monitoring and controlling of pesticides. Researchers have discovered that carbon nanomaterials have a wide range of characteristics such as high porosity, conductivity and easy electron transfer that can be successfully used to detect pesticide residues from food. This review emphasizes the role of carbon nanomaterials in the field of pesticide residue analysis in different food matrices. The carbon nanomaterials including carbon nanotubes, carbon dots, carbon nanofibers, graphene/graphene oxides, and activated carbon fibres are discussed in the review. In addition, the review examines future prospects in this research area to help improve detection techniques for pesticides analysis.
Show more [+] Less [-]A comparison of activated carbon remediation success in floodplain soils contaminated with DDT and its metabolites using ex situ and in situ experimentation
2022
Harwood, Amanda D. | Nutile, Samuel A. | Simpson, Adam M.
Remediation of hydrophobic organic contaminants using activated carbon is an effective means by which to clean up contaminated areas. Predicting remediation success using laboratory experimentation with soil, however, is unclear. Current remediation efforts involving activated carbon addition to floodplain soils downstream of the Velsicol Chemical Corporation Superfund Site (VCCSS) have offered the opportunity to directly compare in situ activated carbon remediation with laboratory experimentation. The objective of the current study was to compare bioaccumulation of DDT, DDD, and DDE (DDX) residues by earthworms (Eisenia fetida) exposed to laboratory-aged (LA) or field-aged (FA) soils from four locations. Samples were evaluated at 0-, 3-, and 9-months post-remediation to determine the ability of laboratory studies to predict in situ remediation. Floodplain soils downstream from the VCCSS were amended with 2% by weight activated carbon in the field and the laboratory, and then aged for 3- or 9-months. At 0-, 3-, and 9-months bioaccumulation assays were conducted with LA and FA soils and tissue concentrations were compared within study sites. In both LA and FA soils, activated carbon caused significant reductions (37.01–92.94%) in bioaccumulated DDX in earthworms. Field-collected worms showed a similar trend in reduction of bioaccumulated DDX, suggesting activated carbon remediation was successful in reducing bioavailable DDX for native organisms within the floodplain soils. The rate of reduction in bioavailable DDX, however, was significantly faster in LA soils (β = −0.189, p < 0.0001) compared to FA soils (β = −0.054, p < 0.0038). Differences in temperature and methods of activated carbon incorporation between LA and FA soils may account for the differences in remediation rate, suggesting laboratory experiments may overpredict the extent or speed in which remediation occurs in the field. Therefore, use of laboratory studies in predicting success of activated carbon remediation may be most effective when conditions mimic field remediation as closely as possible.
Show more [+] Less [-]Per- and polyfluoroalkyl substance (PFAS) retention by colloidal activated carbon (CAC) using dynamic column experiments
2022
Niarchos, Georgios | Ahrens, Lutz | Kleja, Dan Berggren | Fagerlund, Fritjof
Developing effective remediation methods for per- and polyfluoroalkyl substance (PFAS)-contaminated soils is a substantial step towards counteracting their widespread occurrence and protecting our ecosystems and drinking water sources. Stabilisation of PFAS in the subsurface using colloidal activated carbon (CAC) is an innovative, yet promising technique, requiring better understanding. In this study, dynamic soil column tests were used to assess the retardation of 10 classical perfluoroalkyl acids (PFAAs) (C₅–C₁₁ perfluoroalkyl carboxylic acids (PFCAs) and C₄, C₆, C₈ perfluoroalkane sulfonates (PFSAs)) as well as two alternative PFAS (6:2 and 8:2 fluorotelomer sulfonates) using CAC at 0.03% w/w, to investigate the fate and transport of PFAS under CAC treatment applications. Results showed high retardation rates for long-chain PFAS and eight times higher retardation for the CAC-treated soil compared to the non-treated reference soil for the ∑PFAS. Replacement of shorter chain perfluorocarboxylic acids (PFCAs), such as perfluoropentanoic acid (PFPeA), by longer chained PFAS was observed, indicating competition effects. Partitioning coefficients (Kd values) were calculated for the CAC fraction at ∼10³–10⁵ L kg⁻¹ for individual PFAS, while there was a significant positive correlation (p < 0.05) between perfluorocarbon chain length and Kd. Mass balance calculations showed 37% retention of ∑PFAS in treated soil columns after completion of the experiments and 99.7% higher retention rates than the reference soil. Redistribution and elution of CAC were noticed and quantified through organic carbon analysis, which showed a 23% loss of carbon during the experiments. These findings are a step towards better understanding the extent of CAC's potential for remediation of PFAS-contaminated soil and groundwater and the limitations of its applications.
Show more [+] Less [-]Changing bioavailability of per- and polyfluoroalkyl substances (PFAS) to plant in biosolids amended soil through stabilization or mobilization
2022
Zhang, Weilan | Liang, Yanna
Biosolids containing per- and polyfluoroalkyl substances (PFAS) could contaminate the receiving environments once they are land applied. In this study, we evaluated the feasibility of controlling the bioavailability of PFAS in biosolids to timothy-grass through stabilization or mobilization approaches. Stabilization was accomplished by adding a sorbent (i.e. granular activated carbon (GAC), RemBind, biochar) to biosolids, while mobilization was achieved by adding a surfactant, sodium dodecyl sulphate (SDS), to biosolids. The results showed that the ΣPFAS concentration in grass shoots grown in biosolids amended soil treated by GAC or RemBind at 2% was only 2.77% and 3.35% of the ΣPFAS concentration detected in shoots grown in biosolids amended soil without a sorbent, respectively, indicating the effectiveness of GAC and RemBind for stabilizing PFAS and reduce their bioavailability. On the other hand, mobilization by adding SDS to biosolids at a dose range of 10–100 mg/kg significantly increased the plant uptake of ΣPFAS by 15.48%–108.57%. Thus, mobilization by adding SDS could be a valuable approach for enhancing the PFAS removal if phytoremediation is applied. Moreover, higher rate of PFAS uptake took place after grass cutting was observed in this study. Thus, proper mowing and regrowth of timothy-grass could lead to efficient and cost-effective removal of PFAS from biosolids amended soil through phytoremediation and leave the site clean to be used for other purposes.
Show more [+] Less [-]Hierarchically porous biochar templated by in situ formed ZnO for rapid Pb2+ and Cd2+ adsorption in wastewater: Experiment and molecular dynamics study
2022
Wu, Jiawen | Wang, Tao | Shi, Nan | Min, Fanfei | Pan, Wei-Ping
3D hierarchical porous biochar (HPBC) was synthesized by a thermally removable template without post-activation. Zn(NO₃)₂ decomposition produced gases and ZnO in situ to activate and expand the three-dimensional micro-and mesopores. Compared with pristine biochar (BC), the specific surface area and pore volume of HPBC were increased by 223 and 75 times, respectively. The abundant pore structure of HPBC significantly enhanced the diffusion rate of heavy metals. For example, compared to BC, the time required for HPBC to adsorb Pb²⁺ reach adsorption equilibrium was reduced by 87.5% (40 min vs 5min). Such an adsorption performance of HPBC was also insensitive to different background ions (K⁺, Na⁺, Ca²⁺, and Mg²⁺) with a much higher concentration than that of heavy metals. When applied to treat desulfurization wastewater from power plants, HPBC yielded 100% removal of Pb²⁺ and Cd²⁺, much higher than that by using commercial activated carbon (28%). Molecular dynamics simulation revealed different locations preferred by the adsorption of Pb²⁺ (micropores) and Cd²⁺ (mesopores) in the hierarchical pore structures. The adsorption of Pb²⁺ and Cd²⁺ on HPBC was mainly achieved by diffusion, oxygen functional group complexation, and precipitation. These results provided better knowledge to understand the microscopic adsorption mechanisms of heavy metals in hierarchical pores and a facile yet robust strategy to design such structures in biochar for efficient wastewater treatment.
Show more [+] Less [-]Mitigation of hazardous toluene via ozone-catalyzed oxidation using MnOx/Sawdust biochar catalyst
2022
Cha, Jin Sun | Kim, Young-Min | Lee, Im Hack | Choi, Yong Jun | Rhee, Gwang Hoon | Song, Hocheol | Jeon, Byong-Hun | Lam, Su Shiung | Khan, Moonis Ali | Andrew Lin, Kun-Yi | Chen, Wei-Hsin | Park, Young-Kwon
This study investigated catalytic ozone oxidation using a sawdust char (SDW) catalyst to remove hazardous toluene emitted from the chemical industry. The catalyst properties were analyzed by proximate, ultimate, nitrogen adsorption-desorption isotherms, Fourier-transform infrared, and X-ray photoelectron spectroscopy analyses. In addition, hydrogen-temperature programmed reduction experiments were conducted to analyze the catalyst properties. The specific area and formation of micropores of SDC were improved by applying KOH treatment. MnOx/SDC-K3 exhibited a higher toluene removal efficiency of 89.7% after 100 min than MnOx supported on activated carbon (MnOx/AC) with a removal efficiency of 6.6%. The higher (Oₐdₛ (adsorbed oxygen)+Oᵥ(vacancy oxygen))/OL (lattice oxygen) and Mn³⁺/Mn⁴⁺ ratios of MnOx/SDC-K3 than those of MnOx/AC seemed to be important for the catalytic oxidation of toluene.
Show more [+] Less [-]High-efficiency removal of benzene vapor using activated carbon from Althaea officinalis L. biomass as a lignocellulosic precursor
2022
Isinkaralar, Kaan
Benzene is a primary air pollutant commonly found widespread in the indoor environment. It has always been a research focus on the environment due to the causes of significant human health concerns. It has been widely utilized in the synthesis of solvent production, which can rarely be found in high concentrations in outdoor air or high amounts in indoor air, depending on its sources. It is aimed to remove different initial benzene concentrations (from 5 to 1500 ppm) with the production of activated carbon as an excellent adsorbent with a high surface area to be used in these situations. Lignocellulosic wastes have great potential for activated carbon for their advantages (abundant, recycled, and low-cost materials, etc.). This study aimed to evaluate biowaste material for activated carbon production from Althaea officinalis L. biomass by chemical activation (H₂SO₄, LiOH, and ZnCl₂) at temperatures between 500 and 900 °C. Newly developed powdered activated carbons (Ao-ACs) are also tabulated as Ao-AC1-45 for easy reference. Benzene vapor was collected into Tenax TA® tubes by automatic thermal desorption in conjunction with a capillary gas chromatography-mass spectrometry (TD-GC/MS). The significant surface area and production yield of Ao-ACs were obtained at 1424 m²/g (Ao-AC43) and up to 40.32%, respectively. The maximum gas-phase benzene adsorption capacity was 140 mg/g at 270 min. This research has focused on adsorption gas-phase benzene removal onto Ao-ACs as a low-cost adsorbent from the Althaea officinalis L. biomass. Conspicuously, more study is needed to perform the enhanced adsorption of airborne pollutants capacity with inexpensive activated carbon from waste biomass materials.
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