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Enhanced removal of sulfonamide antibiotics by KOH-activated anthracite coal: Batch and fixed-bed studies
2016
Zuo, Linzi | Ai, Jing | Fu, Heyun | Chen, Wei | Zheng, Shourong | Xu, Zhaoyi | Zhu, Dongqiang
The presence of sulfonamide antibiotics in aquatic environments poses potential risks to human health and ecosystems. In the present study, a highly porous activated carbon was prepared by KOH activation of an anthracite coal (Anth-KOH), and its adsorption properties toward two sulfonamides (sulfamethoxazole and sulfapyridine) and three smaller-sized monoaromatics (phenol, 4-nitrophenol and 1,3-dinitrobenzene) were examined in both batch and fixed-bed adsorption experiments to probe the interplay between adsorbate molecular size and adsorbent pore structure. A commercial powder microporous activated carbon (PAC) and a commercial mesoporous carbon (CMK-3) possessing distinct pore properties were included as comparative adsorbents. Among the three adsorbents Anth-KOH exhibited the largest adsorption capacities for all test adsorbates (especially the two sulfonamides) in both batch mode and fixed-bed mode. After being normalized by the adsorbent surface area, the batch adsorption isotherms of sulfonamides on PAC and Anth-KOH were displaced upward relative to the isotherms on CMK-3, likely due to the micropore-filling effect facilitated by the microporosity of adsorbents. In the fixed-bed mode, the surface area-normalized adsorption capacities of Anth-KOH for sulfonamides were close to that of CMK-3, and higher than that of PAC. The irregular, closed micropores of PAC might impede the diffusion of the relatively large-sized sulfonamide molecules and in turn led to lowered fixed-bed adsorption capacities. The overall superior adsorption of sulfonamides on Anth-KOH can be attributed to its large specific surface area (2514 m²/g), high pore volume (1.23 cm³/g) and large micropore sizes (centered at 2.0 nm). These findings imply that KOH-activated anthracite coal is a promising adsorbent for the removal of sulfonamide antibiotics from aqueous solution.
显示更多 [+] 显示较少 [-]Insight into the adsorption of PPCPs by porous adsorbents: Effect of the properties of adsorbents and adsorbates
2016
Zhu, Zengyin | Xie, Jiawen | Zhang, Mancheng | Zhou, Qing | Liu, Fuqiang
Adsorption is an efficient method for removal of pharmaceuticals and personal care products (PPCPs). Magnetic resins are efficient adsorbents for water treatment and exhibit potential for PPCP removal. In this study, the magnetic hypercrosslinked resin Q100 was used for adsorption of PPCPs. The adsorption behavior of this resin was compared with those of two activated carbons, namely, Norit and F400D. Norit exhibited the fastest adsorption kinetics, followed by Q100. Norit featured a honeycomb shape and long-range ordered pore channels, which facilitated the diffusion of PPCPs. Moreover, the large average pore size of Q100 reduced diffusion resistance. The adsorbed amounts of 11 PPCPs on the three adsorbents increased with increasing adsorbate hydrophobicity. For Q100, a significant linear correlation was observed between the adsorption performance for PPCPs and hydrophobicity (logD value) of adsorbates (R2 = 0.8951); as such, PPCPs with high logD values (>1.69) could be efficiently removed. Compared with those of Norit and F400D, the adsorption performance of Q100 was less affected by humic acid because of the dominant hydrophobic interaction. Furthermore, Q100 showed improved regeneration performance, which renders it promising for PPCP removal in practical applications.
显示更多 [+] 显示较少 [-]Investigation and risk evaluation of the occurrence of carbamazepine, oxcarbazepine, their human metabolites and transformation products in the urban water cycle
2016
Brezina, Elena | Prasse, Carsten | Meyer, Johannes | Mückter, Harald | Ternes, Thomas A.
Trace organic contaminants such as pharmaceuticals, personal care products and industrial chemicals are frequently detected in the urban water cycle, including wastewater, surface water and groundwater, as well as drinking water. These also include human metabolites (HMs), which are formed in the human body and then excreted via urine or feces, as well as transformation products (TPs) formed in engineered treatment systems and the aquatic environment. In the current study, the occurrence of HMs as well as their TPs of the anticonvulsants carbamazepine (CBZ) and oxcarbazepine (OXC) were investigated using LC tandem MS in effluents of wastewater treatment plants (WWTPs), surface water and groundwater. Highest concentrations were observed in raw wastewater for 10,11-dihydro-10,11-dihydroxycarbamazepine (DiOHCBZ), 10,11-dihydro-10-hydroxy-cabamazepine (10OHCBZ) and CBZ with concentrations ranging up to 2.7 ± 0.4, 1.7 ± 0.2 and 1.07 ± 0.06 μg L−1, respectively. Predictions of different toxicity endpoints using a Distributed Structure-Searchable Toxicity (DSSTox) expert system query indicated that several HMs and TPs, in particular 9-carboxy-acridine (9-CA-ADIN) and acridone (ADON), may exhibit an increased genotoxicity compared to the parent compound CBZ. As 9-CA-ADIN was also detected in groundwater, a detailed investigation of the genotoxicity of 9-CA-ADIN is warranted. Investigations of an advanced wastewater treatment plant further revealed that the discharge of the investigated compounds into the aquatic environment could be substantially reduced by ozonation followed by granular activated carbon (GAC) filtration.
显示更多 [+] 显示较少 [-]High-throughput profiling of antibiotic resistance genes in drinking water treatment plants and distribution systems
2016
Xu, Like | Ouyang, Weiying | Qian, Yanyun | Su, Chao | Su, Jianqiang | Chen, Hong
Antibiotic resistance genes (ARGs) are present in surface water and often cannot be completely eliminated by drinking water treatment plants (DWTPs). Improper elimination of the ARG-harboring microorganisms contaminates the water supply and would lead to animal and human disease. Therefore, it is of utmost importance to determine the most effective ways by which DWTPs can eliminate ARGs. Here, we tested water samples from two DWTPs and distribution systems and detected the presence of 285 ARGs, 8 transposases, and intI-1 by utilizing high-throughput qPCR. The prevalence of ARGs differed in the two DWTPs, one of which employed conventional water treatments while the other had advanced treatment processes. The relative abundance of ARGs increased significantly after the treatment with biological activated carbon (BAC), raising the number of detected ARGs from 76 to 150. Furthermore, the final chlorination step enhanced the relative abundance of ARGs in the finished water generated from both DWTPs. The total enrichment of ARGs varied from 6.4-to 109.2-fold in tap water compared to finished water, among which beta-lactam resistance genes displayed the highest enrichment. Six transposase genes were detected in tap water samples, with the transposase gene TnpA-04 showing the greatest enrichment (up to 124.9-fold). We observed significant positive correlations between ARGs and mobile genetic elements (MGEs) during the distribution systems, indicating that transposases and intI-1 may contribute to antibiotic resistance in drinking water. To our knowledge, this is the first study to investigate the diversity and abundance of ARGs in drinking water treatment systems utilizing high-throughput qPCR techniques in China.
显示更多 [+] 显示较少 [-]Mercury remediation in wetland sediment using zero-valent iron and granular activated carbon
2016
Lewis, Ariel S. | Huntington, Thomas G. | Marvin-DiPasquale, Mark C. | Amirbahman, Aria
Wetlands are hotspots for production of toxic methylmercury (MeHg) that can bioaccumulate in the food web. The objective of this study was to determine whether the application of zero-valent iron (ZVI) or granular activated carbon (GAC) to wetland sediment could reduce MeHg production and bioavailability to benthic organisms. Field mesocosms were installed in a wetland fringing Hodgdon Pond (Maine, USA), and ZVI and GAC were applied. Pore-water MeHg concentrations were lower in treated compared with untreated mesocosms; however, sediment MeHg, as well as total Hg (THg), concentrations were not significantly different between treated and untreated mesocosms, suggesting that smaller pore-water MeHg concentrations in treated sediment were likely due to adsorption to ZVI and GAC, rather than inhibition of MeHg production. In laboratory experiments with intact vegetated sediment clumps, amendments did not significantly change sediment THg and MeHg concentrations; however, the mean pore-water MeHg and MeHg:THg ratios were lower in the amended sediment than the control. In the laboratory microcosms, snails (Lymnaea stagnalis) accumulated less MeHg in sediment treated with ZVI or GAC. The study results suggest that both GAC and ZVI have potential for reducing MeHg bioaccumulation in wetland sediment.
显示更多 [+] 显示较少 [-]Covalent triazine-based framework: A promising adsorbent for removal of perfluoroalkyl acids from aqueous solution
2016
Wang, Bingyu | Lee, Linda S. | Wei, Chenhui | Fu, Heyun | Zheng, Shourong | Xu, Zhaoyi | Zhu, Dongqiang
Perfluoroalkyl acids (PFAAs) are highly stable, persistent, and ubiquitous in the environment with significant concerns growing with regards to both human and ecosystem health. Due to the high stability to both biological and chemical attack, the only currently feasible approach for their removal from water is adsorbent technology. The main objective of this study was to assess a covalent triazine-based framework (CTF) adsorbent for removal from aqueous solutions of perfluoro C4, C6, and C8 carboxylates and sulfonates including the two C8s most commonly monitored, perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS). Adsorption affinity and capacity were quantified and compared to three commonly used sorbents: pulverized microporous activated carbon, single-walled carbon nanotubes, and Amberlite IRA-400 anion-exchange resin. CTF adsorbent exhibited pronouncedly higher adsorption affinity and capacity of PFAAs than other test sorbents. The remarkably strong adsorption to CTF can be attributed to the favored electrostatic interaction between the protonated triazine groups on the inner wall of the hydrophobic CTF pore and the negatively charged head groups of the PFAAs intercalated between the CTF layers. The homogeneous, nanosized pores (1.2 nm) of CTF hindered adsorption of a large-sized dissolved humic acid, thus minimizing the suppression of PFAA adsorption. Additionally, regeneration of CTF was easily accomplished by simply raising pH > 11, which inhibited the electrostatic adsorptive interaction of PFAAs.
显示更多 [+] 显示较少 [-]Copper(II) and Phenol Adsorption by Cell Surface Treated Candida tropicalis Cells in Aqueous Suspension
2016
Honfi, Krisztina | Tálos, Katalin | Kőnig-Péter, Anikó | Kilár, Ferenc | Pernyeszi, Tímea
An experimental study was performed to determine the feasibility of using physically treated Candida tropicalis cells for sorption of Cu(II) and phenol, the role of competition between phenol molecules and Cu(II). The yeast cells were lyophilized (LC), heat-treated at 65 °C for 24 h (HT1), at 90 °C for 24 h (HT2), and 72 h (HT3), inactivated at 120 °C and 104 kPa for 20 min (PC). The adsorption isotherms were determined in batch system. Experimental equilibrium data were evaluated using Langmuir, Freundlich, and Dubinin–Radushkevich isotherm models by linear and non-linear regression. The adsorbed Cu(II) and phenol amounts by yeast cells were decreased due to the physical treatments of cells. With the increase of biomass dosage from 1 to 10 g L⁻¹, the adsorption efficiency was increased. The Cu(II) adsorption capacity was also determined in the presence of phenol at various initial concentrations, and in these systems, phenol adsorption isotherms were determined. In the presence of phenol, the Cu(II) sorption capacity by lyophilized cells and carbon particles was decreased. The most commonly used sorbent in water treatment is activated carbon with large specific surface; therefore, the results were compared with the experimental data obtained by using activated carbon (AC).
显示更多 [+] 显示较少 [-]Low temperature destruction of PCDD/Fs by catalysis coupled with activated carbon
2016
Yu, Ming-feng | Li, Xiao-dong | Chen, Tong | Lu, Sheng-yong | Yan, Jian-hua
In order to enhance the oxidation and adsorption capacity of catalyst, two kinds of activated carbon (AC) are mechanically mixed with V₂O₅-WO₃/TiO₂ catalyst respectively. In this study, the mixtures (M-1: catalyst mixing with AC based on lignite; M-2: the one on coconut shell) are investigated to destroy high concentration (9.8 ng I-TEQ Nm⁻³) PCDD/Fs at low temperature (160 °C). Adding AC into the catalyst obviously increases removal efficiency (RE) and destruction efficiency (DE). However, M-2 presents higher RE value and lower DE value compared with M-1 at the same conditions as the stronger adsorption capacity of AC based on coconut shell. For the M-2 mixture, RE values are decreasing while DE values show an opposite trend with the ratios of catalyst to AC increasing. Oxygen plays a positive role on the destruction of PCDD/Fs by accelerating the conversion of V⁴⁺Oₓ and V⁵⁺Oₓ. Adjusting oxygen content from 0 to 20 % could increase the DE value from 27.4 to 82.2 % for the M-1 and from 15.8 to 68.9 % for the M-2. In the presence of ozone, a dark brown flock will be generated when the ratio of AC and catalyst is 4:1 due to the reaction between AC and ozone, which results in the lower RE and DE values. The RE and DE values reach the maximum of 96.3 %, 90.6 % in this paper, respectively, when the ratio of AC and catalyst is 1:1 with ozone. Finally, the regenerating of mixture is investigated. Most of dioxin residues in the mixture are desorbed and oxidized by catalysis at 200 °C in the presence of oxygen.
显示更多 [+] 显示较少 [-]Investigating PPCP Removal from Wastewater by Powdered Activated Carbon/Ultrafiltration
2016
Rodriguez, Elena | Campinas, Margarida | Acero, Juan Luis | Rosa, Maria João
Powdered activated carbon/ultrafiltration (PAC/UF) hybrid process was investigated for removing from wastewater five pharmaceutical and personal care products (PPCPs): 1-H-benzotriazole, DEET, chlorophene, 3-methylindole and nortriptyline-HCl. Adsorption, UF and PAC/UF experiments were performed, focusing on PPCP adsorption as a function of PPCP characteristics and organic matter (EfOM) competition. Two water matrices and two fine-particle PACs were studied, differing on EfOM nature and concentration and on PAC microporosity. Neutral PPCP uptake by the positively charged, meso- and microporous PACs followed PPCP hydrophobicity expressed by log Kₒw. The uptake of the positively charged nortriptyline exceeded the expected from log D due to its high aromaticity and the background ions, which partially shielded PAC-nortriptyline electrostatic repulsions. Adsorption capacity depended on PPCP hydrophobicity whereas the kinetics further depended on PPCP charge. Hydrophobic EfOM was preferentially adsorbed and a stronger competitor, particularly for PPCPs with logKₒw < 2.6. The highly microporous PAC better adsorbed these PPCPs and the hydrophobic EfOM, and it attenuated the EfOM competition. For all waters, PAC had no effect on UF-flux, and it significantly improved PPCP and EfOM removal by PAC/UF over standalone PAC and UF. For all conditions and microcontaminants, PPCP uptake exhibited a sigmoid curve with logKₒw, with a turning point at 2.2–2.6. In real applications, meso- and highly microporous PACs are recommended, and the dose should target the PPCPs with log Kₒw < 2.6.
显示更多 [+] 显示较少 [-]Synthesis, Characterization and Application of ZrCl4-Graphene Composite Supported on Activated Carbon for Efficient Removal of Fluoride to Obtain Drinking Water
2016
Marin, Pricila | Módenes, Aparecido Nivaldo | Bergamasco, Rosângela | Paraíso, Paulo Roberto | Hamoudi, Safia
The aim of this study is to evaluate the fluoride removal from contaminated water using a new adsorbent material of high efficiency to obtain drinking water. The ZrCl₄-graphene supported on vegetal activated carbon composite (G-ZrCl₄/VAC) was synthesized and characterized using transmission and scanning electron microscopy, N₂ physisorption, energy dispersive X-ray spectrometry, Fourier transform-infrared spectroscopy, X-ray diffraction, and Raman spectroscopy. Furthermore, the point of zero charge was determined. The G-ZrCl₄/VAC was evaluated for fluoride adsorptive removal from water under several operating conditions in batch system. The results indicated that fluoride adsorption by G-ZrCl₄/VAC is favored at low pH values with the maximum adsorption at pH 2, corresponding to 97.22% removal. Among the conditions of temperature and agitation evaluated, the best results were achieved at 30 °C and 130 rpm, with removal percentages equal to 47.78 and 48.48%, respectively. The equilibrium of the system was achieved in 5 h of operation. The pseudo-first order kinetic model was the one that best described the kinetic data, while the equilibrium data were best described by the Langmuir isotherm with maximum adsorption capacity equal to 3.89 mg g⁻¹. Therefore, the results obtained show that the material synthesized has a great capacity for adsorption and demonstrate the viability of use of G-ZrCl₄/VAC in the removal of fluoride to obtain drinking water.
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