SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Jiaxin Xu,Jing Zou,Jianying Wu,Huiping Zeng,Yixin Huang,Jingxin Yang,Chunming Gong,Siying Chen,Jun Ma
Chlorination, one of the most common oxidation strategies, performed limited degradation capacity towards many emerging organic contaminants under neutral pH conditions. In this study, 2,2′-azinobis(3-ethylbenzothiazoline)-6-sulfonate (ABTS) was discovered to possess an outstanding activation property towards free available chlorine (FAC) during the chlorination of diclofenac (DCF) among pH 6.0–9.5. ABTS radical (ABTS •+ ) primarily accounted for the elimination of DCF in the ABTS/FAC system, although hydroxyl radicals , reactive chlorine species, and singlet oxygen were also generated via the self-decomposition of FAC. ABTS acted as the electron shuttle to degrade DCF in the ABTS/FAC system, where ABTS was firstly oxidized by FAC to ABTS •+ via single electron transfer , and followed by the elimination of DCF with the generated ABTS •+ . Eight DCF degradation intermediates were identified by LC/Q-TOF/MS, and four DCF degradation pathways were proposed. Real water bodies, humic acid , and the coexistent anions of Cl − , HCO 3 − , NO 3 − , and SO 4 2− performed negligible influence on DCF removal in ABTS/FAC system. ABTS/FAC system was much superior to sole chlorination in terms of toxicity reduction and anti-interference capacity. Overall, this study innovatively introduced ABTS as the electron shuttle to enhance the oxidative capacity of FAC under neutral pH conditions and provided a new insight that the ABTS-like organic/synthetic components might play an important role in degrading emerging organic contaminants by chlorination in water treatment .
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高影响因子
RSC Advances
·
2021
·Vol. 11
·期 12
·6804-6817
·
IF 3.361
Yunlan Peng,Hongle Shi,Zhenran Wang,Yongsheng Fu,Yiqing Liu
Diclofenac (DCF) is a common non-steroidal anti-inflammatory drug, which is frequently detected in different environmental media such as surface water, groundwater, domestic sewage, and sediment. In this study, UV-activated peroxymonosulfate (PMS) was used to degrade DCF by generating active radicals (i.e., SO4˙− and HO˙) with strong oxidizing properties. The effects of PMS dosage, pH, initial DCF concentration and common water constituents on the removal of DCF as well as its degradation mechanism in UV/PMS system were investigated. Compared to UV alone and PMS alone systems, DCF was removed more efficiently in the UV/PMS system at pH 7.0 due to the contribution of SO4˙− and HO˙, and its degradation followed the pseudo-first order kinetic model. As the dosage of PMS or solution pH increased, the degradation efficiency of DCF was gradually enhanced. The highest DCF degradation was obtained at pH 11.0 in this study, because the molar absorption coefficient of PMS increased with increasing pH at 254 nm resulting in generation of more reactive radicals at high pH. Removal efficiency of DCF was decreased significantly with the increase in its initial concentration due to the insufficient concentration of radicals. The presence of HCO3− and NO3− could promote the degradation of DCF because of the role of carbonate radicals and extra HO˙ formed, respectively, while NOM inhibited DCF degradation due to its competition with DCF for reactive radicals. No obvious influence on DCF degradation was observed in the UV/PMS system with the addition of Cl− and SO42−. The degradation of DCF by UV/PMS in real waters was slightly suppressed compared with its removal in ultrapure water. Seven transformation products were detected using UPLC-QTOF/MS, and the potential degradation mechanism of DCF was thus proposed showing six reaction pathways including hydroxylation, decarboxylation, dechlorination–cyclization, formylation, dehydrogenation and dechlorination–hydrogenation.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Ying-Ying Jiang,Zi-Wen Chen,Man-Man Li,Qiu-Hong Xiang,Xi-Xi Wang,Heng-Feng Miao,Wen-Quan Ruan
A nano-calcium peroxide (nCaO 2 ) powder with a purity of 89.1% was prepared using an improved traditional method. Then, the as-prepared nCaO 2 was used as the source of hydrogen peroxide (H 2 O 2 ) for the Fenton-like degradation of diclofenac sodium (DCF). The results showed that nCaO 2 performed better for DCF removal when compared to nCaO 2 prepared by a conventional method and commercial calcium peroxide (CaO 2 ). Further experimental results indicated that 97.5% of DCF could be removed in 180 min at a nCaO 2 /Fe 2+ -EDTA/DCF molar ratio of 16/8–8/1, which was more efficient than in the H 2 O 2 /EDTA-Fe 2+ /DCF and nCaO 2 /Fe 2+ /DCF systems. The best removal rate of DCF was at pH 6.0, unlike previous claims that stated that the lower the pH in the buffer system, the better the degradation of DCF. In addition, the influence of water quality parameters, such as Cl − , NO 3 − , SO 4 2− , HCO 3 − , and humic acid (HA), on DCF removal were evaluated. A free radical masking experiment revealed the existence of hydroxyl radical ( OH), superoxide radical (O 2 − ) and singlet oxygen ( 1 O 2 ), and indicated that the degradation of DCF was mainly due to oxidation caused by OH. Electron paramagnetic resonance (EPR) studies for different systems and different active oxygen species were carried out, and it was further confirmed that OH radicals have high intensity in the Fenton-like system based on nCaO 2 . EPR results also showed that the addition of EDTA can promote the production of OH. According to the identification of the dominant reactive species and GC–MS, the possible theoretical DCF degradation pathways were proposed.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2021
·Vol. 29
·期 10
·3401-3411
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IF 3.667
Ye Xiaoxia,Li Yun,Lin Huiting,Chen Yichong,Liu Minghua
Diclofenac sodium, as a typical deputation of non-steroidal anti-inflammatory drugs, is widely used in clinical treatment. Due to the heavy use, diclofenac sodium is commonly detected in water environment, and the removal of diclofenac sodium from wastewater is important for environmental protection. Notably, magnetic separation technology has become a novel performance in the removal of organic pollutants from wastewater in recent years. Herein, we engineered a lignin-based magnetic nanoparticle adsorbent (LMNA) by loading a magnetic core (Fe 3 O 4 ) onto alkali lignin. This novel adsorbent has the advantage of green synthesis and low cost, making it an ideal material for wastewater treatment. Remarkably, the BET surface area of LMNA (739.2 m 2 g −1 ) was higher than that of alkali lignin (2.2 m 2 g −1 ). Adsorption batch experiments confirmed that the LMNA exhibited good adsorption performance to diclofenac sodium with a higher adsorption capacity of 106.4 mg g −1 . The adsorption kinetic data and isothermal were well fitted by the pseudo-second-order rate equation (R 2 = 0.980) and the Langmuir equation (R 2 = 0.991), respectively. Moreover, the reaction mechanisms between the diclofenac sodium and LMNA mainly related to the synergism of electrostatic attractions, π–π stacking interactions and hydrogen bonding interactions. Especially, the LMNA exhibited high magnetic saturation strength (10.5 emu g −1 ) which made it easy to recycle, showing excellent reusability (4 cycles). Our work might introduce significant theoretical and experimental basis for realizing excellent adsorption of emerging organic pollutants from wastewater by the magnetic nanoparticle adsorbent. Graphic Abstract
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2020
·
IF 4.872
Matthew Nkoom,Guanghua Lu,Jianchao Liu,Huike Dong
The uptake and depuration kinetics of diclofenac and carbamazepine alone at an environmentally relevant nominal concentration of 2 μg/L and in combination at a concentration ratio of 1:1 with total concentration of 4 μg/L were evaluated in Carassius carassius after 7 d uptake and depuration . Also, the biochemical effects of both drugs alone at nominal concentrations of 2 and 10 μg/L as well as in combination with total concentrations of 4 and 20 μg/L were investigated in Carassius carassius after 7 d exposure followed by 10 d recovery. In the single treatments, steady-state BCFs measured after the 7 d exposure were 73.05, 49.71, 38.01 and 24.93 L/kg for diclofenac and 9.25, 8.99, 5.29 and 4.11 L/kg for carbamazepine in the liver, brain, gill and muscle of Carassius carassius, respectively. Comparatively lower BCFs were measured in the tissues of Carassius carassius for both drugs in the combined treatments. Acetylcholinesterase activity in the brain was significantly induced by diclofenac while carbamazepine and the mixtures significantly inhibited it during all the exposure days as well as after the 10 d recovery in all treatments. This indicates that Carassius carassius could not recover from the neurotoxic effects caused by carbamazepine unlike the inductive effect caused by diclofenac which was recoverable after 10 days. A significant increase in the activities of 7-ethoxyresorufin O-deethylase and glutathione s-transferase for individual and mixed pharmaceuticals suggest that metabolism and detoxification of both drugs took place in the liver of Carassius carassius . Also, a significant increase in the activities of superoxide dismutase, catalase , glutathione reductase and malondialdehyde contents in the individual and mixture treatments mean that the antioxidant defence system of Carassius carassius was triggered to fight against oxidative stress but lipid peroxidation still occurred. However, Carassius carassius recovered from all these increases (superoxide dismutase, catalase, glutathione reductase and malondialdehyde) after the 10 d recovery, suggesting that oxidative damage is reversible. Our results indicate that both drugs at environmentally relevant concentrations might cause adverse effects in Carassius carassius and other fish species.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Lanbo Bi,Zhonglin Chen,Linghan Li,Jing Kang,Shengxin Zhao,Binyuan Wang,Pengwei Yan,Yabin Li,Xiaoxiao Zhang,Jimin Shen
In the paper, molecularly imprinted TiO 2 was prepared by surface molecularly imprinted technology and liquid phase deposition method for preferential removal of persistent toxic pollutants from complex environmental water. Diclofenac was selected as the template molecule and target for photodegradation study. The characterization results of SEM , TEM, FTIR and XRD showed that the TiO 2 film with imprinted diclofenac was successfully synthesized on the surface of TiO 2 particles. Meanwhile, the adsorption and photodegradation experiments also indicated that the molecularly imprinted TiO 2 had larger adsorption capacity, better selectivity and higher photodegradation performance for diclofenac than non-imprinted TiO 2 . The primary active species and degradation pathways during photodegradation process were also elucidated according to radical capture experiments and UPLC-MS-TOF technology. The prepared molecularly imprinted TiO 2 has the advantages of efficient removal ability, high stability and environmental protection, so it has a wide application value in water treatment and water environmental restoration, especially when involved persistent toxic pollutants.
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ACS Omega
·
2019
·
IF 2.584
Naqing Mao,Lijin Huang,Qin Shuai
In this work, a series of porous carbon materials (PCs) were obtained at different carbonization temperatures (800, 900, 1000, and 1100 °C) by a simple and fast solvent-free method. Moreover, the feasibility of PCs as reliable and efficient adsorbents to capture diclofenac sodium (DCF) from the water was evaluated. Notably, porous carbon (PC) prepared at 1000 °C (PC-1000) was found to be the best candidate for the adsorption of DCF. Remarkably, adsorption equilibrium was achieved within 3 h, which followed a pseudo-second-order kinetic model with a high correlation coefficient (R2 > 0.994). Furthermore, experimental data obtained from adsorption isotherm indicated that the capture of DCF onto PC-1000 followed the Langmuir adsorption model (R2 > 0.997), wherein its maximum adsorption capacity was calculated to be 392 mg/g. In addition, based on the results obtained from the zeta potential of PC-1000 under different pH and the adsorbed quantity of DCF along with functional groups created on the surface of PC-1000, electrostatic and H-bonding interactions were proposed as the possible adsorption mechanisms. Due to its high stability and excellent reusability, PC-1000 has been testified as a promising candidate for removing DCF from contaminated water.
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CHEMOSPHERE
·
2019
·
IF 5.108
Hongbin Wang,Shixiang Wang,Yiqing Liu,Yongsheng Fu,Peng Wu,Gaofeng Zhou
As an emerging pollutant, Diclofenac (DCF) has potential threats to ecosystem and human health, and it can hardly be removed by conventional wastewater treatment processes . In this study, Fe(II)-activated bisulfite (BS), an advanced oxidation process , was used for rapid removal of DCF. The effect of initial pH, Fe(II) dosage, BS concentration, dissolved oxygen and reaction temperature on DCF removal and its degradation mechanism were investigated. Compared to Fe(II)/persulfate system, the removal efficiency of DCF was higher by Fe(II)/BS, and its degradation followed pseudo-first order kinetic model. Due to the morphology of Fe(II) and BS, the optimal pH for DCF degradation was 4.0. The increased initial Fe(II) or BS concentration promoted DCF degradation while excess Fe(II) or BS caused an inhibition effect as a SO 4 − scavenger. Dissolved oxygen was an essential factor inducing the conversion of SO 3 − to SO 4 − , while it had no effect on DCF removal in the range of 4.6–8.3 mg L −1 . The activation energy of this reaction was calculated to be 120.75 ± 3.43 kJ mol −1 based on the improved DCF degradation with increasing temperature. According to the radical scavenging experiments, the contribution of SO 4 − , HO and the other reactive species to DCF degradation in Fe(II)/BS system were 71.1%, 24.6% and 4.3%, respectively. Nine transformation products were detected using UPLC-Q-TOF-MS. The potential degradation mechanism of DCF was thus proposed showing five reaction pathways including hydroxylation, decarboxylation , dehydration, dechlorination and formylation.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Shuting Zhuang,Rong Cheng,Jianlong Wang
UiO-66 type metal organic frameworks (MOFs), including UiO-66 and UiO-66-NH 2 , were synthesized, characterized, and applied for the adsorptive removal of diclofenac (DCF) from aqueous solutions. The effect of synthetic conditions (e.g., different linkers and activation temperatures) and adsorptive conditions (e.g., contact time, initial concentration, temperature, and pH) on DCF removal was examined. UiO-66-NH 2 showed a higher adsorption capacity than UiO-66, and the increase of activation temperature can improve the adsorption capacity of UiO-66-NH 2 towards DCF. The adsorption of DCF by UiO-66-NH 2 was endothermic and almost not affected by pH in the range of 4.8–7.7. The adsorption of DCF onto UiO-66 type MOFs conformed to the pseud second-order kinetic model and the Langmuir isothermal model, with adsorption capacity of 357 mg g −1 for UiO-66 and 555 mg g −1 for UiO-66-NH 2 . Electrostatic interaction and H-bonding possibly played a vital role for DCF adsorption. The as-prepared UiO-66 type MOFs were efficient adsorbent for DCF removal from aqueous solution.
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CHEMOSPHERE
·
2018
·
IF 4.427
Xue Xue Liang,A.M. Omer,Zhao-hong Hu,Yang–guang Wang,Di Yu,Xiao-kun Ouyang
In this study, we prepared a magnetic composite based on amine-functionalized chitosan (aminochitosan; AmCS) and Fe 3 O 4 to remove diclofenac sodium (DS) from water. The fabricated AmCS@Fe 3 O 4 composite was characterized using Fourier-transform infrared spectroscopy, transmission electron microscopy , scanning electron microscopy, vibrating sample magnetometry, X-ray diffraction, and thermogravimetric analysis . Furthermore, we investigated the influence of pH, initial DS concentration, and adsorbent dosage on the adsorption of DS. Through thermodynamic analysis, we found that the data corresponded with the Langmuir adsorption isotherm model. The maximum adsorption capacity reached 469.48 mg g −1 , and the adsorption process followed the pseudo-second-order kinetic model. Finally, the AmCS@Fe 3 O 4 composite retained good adsorption characteristics after four consecutive cycles, with removal efficiency exceeding 70%. Therefore, the developed adsorbent could be used for efficient adsorptive removal of trace drugs and personal care products from water bodies.
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CHEMOSPHERE
·
2016
·
IF 3.698
Xian Lu,Yisheng Shao,Naiyun Gao,Juxiang Chen,Yansen Zhang,Qiongfang Wang,Yuqi Lu
This study demonstrates the use of MIEX resin as an efficient adsorbent for the removal of clofibric acid (CA) and diclofenac (DCF). The adsorption performance of CA and DCF are investigated by a batch mode in single-component or bi-component adsorption system. Various factors influencing the adsorption of CA and DCF, including initial concentration, contact time, adsorbent dosage, initial solution pH, agitation speed, natural organic matter and coexistent anions are studied. The Langmuir model can well describe CA adsorption in single-component system, while the Freundlich model gives better fitting in bi-component system. The DCF adsorption can be well fitted by the Freundlich model in both systems. Thermodynamic analyses show that the adsorption of CA and DCF is an endothermic (ΔH o > 0), entropy driven (ΔS o > 0) process and more randomness exists in the DCF adsorption process. The values of Gibbs free energy (ΔG o < 0) indicate the adsorption of DCF is spontaneous but nonspontaneous (ΔG o > 0) for CA adsorption. The kinetic data suggest the adsorption of CA and DCF follow the pseudo-first-order model in both systems and the intra-particle is not the unique rate-limiting step. The adsorption process is controlled simultaneously by external mass transfer and surface diffusion according to the surface diffusion modified Biot number (Bi s ) ranging from 1.06 to 26.15. Moreover, the possible removal mechanism for CA and DCF is respectively proposed based on the ion exchange stoichiometry .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yanxin Gao,Ting Cheng,Fankang Zhao,Guocheng Huang,Jinhong Bi
The treatment of emerging contaminants is essential but challenging. Herein, a novel MOF/PAN fibrous composite (TCPP@UiO-66/PAN) was synthesized and used as a self-cleaning membrane for the efficient removal of a typical emerging contaminant, diclofenac sodium (DF). The introduction of the secondary linker tetra(4-carboxyphenyl)porphyrin (TCPP) served to expand the pores and enhance its photocatalytic activity. TCPP@UiO-66/PAN shows higher adsorption capacity and initial adsorption rate than UiO-66/PAN. The maximum adsorption capacity of DF on TCPP@UiO-66/PAN reached 202 mg/g by Langmuir model. The DF adsorption mechanism involves the π-π/anion-π interaction, Lewis acid-base interaction, and hydrogen bonding. Based on the dynamic filtration experiment, TCPP@UiO-66/PAN exhibited a remarkable treatment capacity for DF-contaminated water, measuring 3.75 × 10 4 kg/kg. Given its fibrous membrane structure, TCPP@UiO-66/PAN could be easily separated from water and reused. In-situ photo-regeneration emerged as a highly effective method for regenerating TCPP@UiO-66/PAN after reaching adsorption saturation, with over 95 % DF degradation achieved under sunlight irradiation. The decomposition of DF primarily resulted from the generation of h + and 1 O 2 . Additionally, TCPP@UiO-66/PAN exhibited notable antibacterial properties when exposed to visible light. In vitro cytotoxicity assessments further confirmed the safety of these MOF/PAN composites. Combining the advantages of hybrid-linker strategy and fibrous composite, this work provided new insight into constructing MOF-based functional material for wastewater purification.
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