JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2022
·Vol. 31
·期 3
·1129-1143
·
IF 4.705
Tang Qi,Qiu Chongpeng,Zhang You,Zhang Xuefeng,Yuan Zihui,Tan Hailu,Wang Lei,de Hoop Cornelis F.,Qi Jinqiu,Huang Xingyan
In this work, a novel nanocellulose/alum/chitosan/polyethyleneimine biohybrid aerogel (NACPBA) beads adsorbent was successfully prepared to remove diclofenac sodium (DS) from wastewater. The NACPBA beads adsorbent was characterized using Fourier transform infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, X-ray diffractometer, and Brunauer–Emmett–Teller. A possible adsorption mechanism was also discussed. The experimental results showed that the adsorption process was followed by a pseudo-second-order kinetic model and Sips isotherm model with the calculated maximum adsorption capacity of 321.3 mg/g on DS. It was much higher than most of the previously reported works. The adsorption capacity of NACPBA beads on DS was increased rapidly within 120 min, especially in the first 60 min. Furthermore, after five regeneration cycles, NACPBA still retained a good adsorption capacity of 103.7 mg/g with a removal efficiency of 50%. Moreover, 95.4% of DS was removed from river water (simulated 5 mg/L DS-contaminated wastewater). The possible adsorption mechanism was primarily governed by electrostatic attractions and hydrogen bond interactions.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Jia Xie,Minghua Liu,Miao He,Yifan Liu,Jian Li,Fangxia Yu,Yuancai Lv,Chunxiang Lin,Xiaoxia Ye
Developing safe and efficient diclofenac sodium (DS) removal technology has become a critical issue. This study synthesized the fish-scale biochar by co-pyrolysis of fish scale and phosphoric acid (H 3 PO 4 ). In addition to increasing the specific surface area and pore volume of fish-scale biochar, H 3 PO 4 assisted in the formation of Graphitic N and sp 2 C, as well as reacting with C═O groups to form a significant number of phosphorus-containing groups. All these functional groups could act as major active sites for DS adsorption. Adsorption data could well fit pseudo-second-order and Langmuir models. The maximum adsorption capacity of FSB 600-15 for DS was 967.1 mg g −1 , which was much better than that reported in the literature. Under the synergistic effect of various mechanisms (pore-filling effect, electrostatic attraction, H-bonding, π-π, and n-π electron donor-acceptor interactions), the DS ultra-efficient adsorption on FSB 600-15 was realized. Meanwhile, the DS adsorption by FSB 600-15 was an endothermic, spontaneous, and entropy-increasing process. Furthermore, the DS adsorption capacity was more than 426.5 mg g −1 in the actual water, which was sufficient for practical applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 39
·58963-58979
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IF 5.19
Nkoom Matthew,Lu Guanghua,Liu Jianchao
The chronic toxicity of diclofenac (DCF) and carbamazepine (CBZ) as separate substances and in conjunction with their mixture on Daphnia magna was assessed in the parental (F0) and first filial (F1) generations. The second (F1–B2) and fifth (F1–B5) broods of F1 offspring were investigated and compared. Both drugs and their mixture were exposed to each generation of Daphnia magna for 21 days with life history, behavioural and gene expressions as measured endpoints. After the parental exposure, offspring from these two broods were transferred to a clean medium for a 21-day recovery. Exposure to diclofenac, carbamazepine and their mixture significantly inhibited growth, reproduction, swimming activities, heart rate, thoracic limb activities, reproductive and antioxidant-related genes in the parental as well as the first filial generations. These effects were relatively greater in the F1 generation. This indicates that Daphnia magna ’s sensitivity improved while its fitness declined over the two generations, which is an indicator of greater energy requirements for maintenance. Besides, the significant inhibition in the antioxidant-related genes implies that oxidative stress occurred in Daphnia magna under the exposure to these drugs. The significant reduction in the reproductive output, moulting frequency and cyp314 gene expression as a result of exposure to CBZ simultaneously obtained herein may indicate that this drug could act as an endocrine disruptor. Most of these significant effects were not recoverable after the 21-day recovery period. The findings reported herein highlight the necessity to include maternal effects in environmental risk assessment processes, considering that pollutant effects are underestimated during single-generational exposure.
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Pharmaceutics
·
2021
·Vol. 13
·期 3
·338
·
IF 6.321
Ahmed M. Omer,Maha S. Ahmed,Gehan M. El-Subruiti,Randa E. Khalifa,Abdelazeem S. Eltaweil
To develop an effective pH-sensitive drug carrier, alginate (Alg), carboxymethyl chitosan (CMCs), and aminated chitosan (AmCs) derivatives were employed in this study. A simple ionic gelation technique was employed to formulate Alg-CMCs@AmCs dual polyelectrolyte complexes (PECs) microcapsules as a pH-sensitive carrier for efficient encapsulation and release of diclofenac sodium (DS) drug. The developed microcapsules were characterized by Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analyzer (TGA), and scanning electron microscope (SEM). The results clarified that formation of dual PECs significantly protected Alg microcapsules from rapid disintegration at colon conditions (pH 7.4), and greatly reduced their porosity. In addition, the dual PECs microcapsules can effectively encapsulate 95.4% of DS-drug compared to 86.3 and 68.6% for Alg and Alg-CMCs microcapsules, respectively. Higher DS-release values were achieved in simulated colonic fluid [SCF; pH 7.4] compared to those obtained in simulated gastric fluid [SGF; pH 1.2]. Moreover, the drug burst release was prevented and a sustained DS-release was achieved as the AmCs concentration increased. The results confirmed also that the developed microcapsules were biodegradable in the presence of the lysozyme enzyme. These findings emphasize that the formulated pH-sensitive microcapsules could be applied for the delivery of diclofenac sodium.Keywords:alginate;carboxymethyl chitosan;aminated chitosan;pH-sensitive microcapsules;polyelectrolyte complex;drug release
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 7
·1-10
·
IF 5.833
Li Jingxian,Shan Xueling,Jiang Ding,Wang Wenchang,Xu Fangmin,Chen Zhidong
The combination of localized surface plasmon resonance (LSPR) and electrochemiluminescence (ECL) can be an effective way to amplify the signal intensity. In this work, an ECL aptasensor with 3,4,9,10-perylenetetracarboxylic acid–decorated cobalt phosphate (denoted as PTCA/CoP) as the ECL emitter and Au nanoparticles (NPs) as plasma was proposed for diclofenac assay. The prepared PTCA/CoP with special 1D/2D structure exhibited good ability and excellent ECL performance. The diclofenac aptamer acted as a bridge to link the PTCA/CoP and Au NPs; thus, the ECL performance of PTCA/CoP was greatly improved due to the plasma effect of Au NPs. Besides, it was found that the ECL signal of the aptasensor was obviously quenched by the introduction of diclofenac, which might be due to the transformation from the LSPR process to the resonance energy transform (RET) process. Under optimal conditions, the difference of ECL intensity was negatively correlated with the concentration of diclofenac in the range 0.1 pM to 10 μM with a low detection limit of 0.072 pM at the potential of −1.8 V vs. Ag/AgCl ( S / N = 3). The aptasensor was proved to be suitable for the detection of diclofenac in real samples, suggesting its great practicability. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ruoyu Deng,Qiang He,Dongxu Yang,Qi Dong,Jiali Wu,Xiangyu Yang,Yi Chen
Dielectric barrier discharge (DBD) is an attractive advanced oxidation process (AOP) due to its operational convenience and environmental friendliness. However, DBD plasma suffers from relatively low energy utilization, which limits its commercial application. In this study, nano-Fe 0 -CeO 2 is successfully synthesized and used for DBD plasma degradation of diclofenac (DCF). The results show that the nano-Fe 0 -CeO 2 significantly enhances the removal of DCF. A DBD-Fe 0 -CeO 2 system degrades 96.4% DCF within 10 min, which is higher than the DBD system alone (45.8%). The synergistic factor of the DBD system and nano-Fe 0 -CeO 2 reaches 3.731. In addition, the composite catalyst shows ideal reusability. Substance activity and production experiments show that reactive oxygen species (ROS), especially OH, play a key role in the degradation of DCF. Nano-Fe 0 -CeO 2 has synergistic effects with O 3 and H 2 O 2 and significantly promotes the generation of ROS in the DBD system. Based on the intermediates detected by liquid chromatography-mass spectrometry, a reasonable degradation pathway of DCF is proposed. Our findings are helpful for understanding the mechanism of DCF degradation by coupling nano-zero-valent-iron-based nanocomposites in a DBD system; they also provide an effective system for the treatment of refractory organic pollutants in water.
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ACS ES&T Engineering
·
2023
·
IF 7.1
Beiping Zhang,Chaoting Guan,Qin Guo,Run Huang,Jin Jiang
Electrochemical technologies and permanganate oxidation are two attractive strategies in water treatment due to their low cost, easy operation, good adaptability, and environmental friendliness. Interestingly, recent studies have demonstrated that the combination of electrolysis and Mn(VII) (E-Mn(VII) process) shows a synergetic effect on organic contaminants degradation. However, the underlying mechanism of the E-Mn(VII) process remains unclear. In this study, the enhanced removal of diclofenac (DCF) by the E-Mn(VII) process was also demonstrated, and the main reactive species were reidentified. It was found that H2O2 was considerably formed via the reduction of O2 on the cathode, and it played a key role in facilitating Mn(VII) transformation into MnO2. Increasing O2 concentration, working potential, and pH value were conducive to H2O2 formation as well as Mn(VII) transformation to MnO2. Higher Mn(VII) dosages did not impact H2O2 formation but also led to faster MnO2 formation. The enhanced formation of MnO2 was favorable for the fast degradation of DCF in the E-Mn(VII) process owing to the catalytic effect of MnO2 on Mn(VII) oxidation. This was confirmed by the observation that (i) the E-Mn(VII) process showed a similar pH-dependent oxidation trend to that of MnO2 catalytic oxidation of Mn(VII) (i.e., the reactivity was much stronger at lower pH); and (ii) the addition of MnO2 prepared ex situ had a significant enhancing effect on DCF oxidation by the E-Mn(VII) process. Moreover, the possible contribution of reactive manganese intermediates such as soluble free Mn(III), Mn(VI), and Mn(V) was ruled out by the results of the probe experiments, UV–visible spectrophotometry, and examining the reactivity of Mn(III) complexes prepared ex situ. Also, the results of radical scavenging experiments indicated the negligible contribution of HO•. Furthermore, for the practical application of the E-Mn(VII) process in water decontamination, suitable operating parameters (e.g., a moderate potential and relatively lower pH) should be determined to avoid the fast loss of Mn(VII) and the electrical energy consumption. Overall, this work brings new insights into the reaction mechanism of the E-Mn(VII) process as well as proposes an efficient, sustainable, and feasible strategy for water and wastewater treatment.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 6
·5704-5712
·
IF 2.914
Nkoom Matthew,Lu Guanghua,Liu Jianchao,Dong Huike,Yang Haohan
The non-steroidal anti-inflammatory drug (NSAID) diclofenac is one of the most frequently studied as well as controversially discussed pharmaceutically active drug on the subject of its relevance to the environment. This study was conducted to assess the bioconcentration potential of diclofenac and its behavioral and biochemical effects in Daphnia magna . The bioconcentration factors of diclofenac determined after 48 h of aqueous exposure in Daphnia magna were 70.94 and 8.02 for the nominal exposure concentrations of 5 and 100 μg/L, respectively. Diclofenac exposure obviously decreased the filtration and ingestion rates of the daphnids. A significant increase of the acetylcholinesterase activity that was observed in this study indicates that diclofenac might not have neurobehavioral toxicity in Daphnia magna . Significant induction of malondialdehyde content is an indication of overproduction of reactive oxygen species leading to oxidative damage in daphnids after diclofenac exposure. Moreover, significant inhibition of the superoxide dismutase, catalase, and glutathione reductase activities implies that the antioxidant defense system of Daphnia magna was overwhelmed. Also, significant inhibition of glutathione s-transferase activity might point to the fact that the enzyme was not capable to detoxify diclofenac in Daphnia magna . These findings indicate that diclofenac can accumulate and consequently stimulate behavioral and biochemical disturbances in Daphnia magna .
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Catalysts
·
2024
·Vol. 14
·期 10
·687
·
IF 3.8
Na Zhang,Yudong Huo,Chun Pei,Ying Zhang,Lijie Xu,Lu Gan
Percarbonate (SPC) as a promising substitute for liquid H2O2has many advantages in the application of in situ chemical oxidation (ISCO). Developing efficient, cost effective and environmentally friendly catalysts for SPC activation plays the key role in promoting the development of SPC-based ISCO. Herein, the walnut shell biomass was combined with ferric nitrate for the catalytic synthesis of Fe3C@biochar composite (Fe3C@WSB), which demonstrated high efficiency in activating SPC for the removal of diclofenac (DCF). The Fe3C showed average crystallite size of 32.6 nm and the composite Fe3C@WSB demonstrated strong adsorptivity. The prepared Fe3C@WSB could activate both SPC and H2O2with high efficiency at ca. pH 3 with extremely low leaching of iron, while in a weak acidic condition, higher efficiency of DCF removal was obtained in the Fe3C@WSB/SPC process than in the Fe3C@WSB/H2O2process. Moreover, the Fe3C@WSB/SPC and Fe3C@WSB/H2O2processes did not show significant differences when supplied with varying amounts of catalyst or oxidant, but the Fe3C@WSB/SPC process exhibited stronger capability in dealing with relatively highly concentrated DCF solution. Based on quenching experiments and electron spin resonance (ESR) analysis, heterogeneous activation of SPC was assumed as the dominant route for DCF degradation, and both the oxidation by radicals, including •OH, •O2−and CO3•−, combined with electron transfer pathway contributed to DCF degradation in the Fe3C@WSB/SPC process. The cycling experiment results also revealed the stability of Fe3C@WSB. This work may cast some light on the development of efficient catalysts for the activation of SPC.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ge Song,Yang Zheng,Minghua Zhou
The application of bimetallic catalysts in heterogeneous electro-Fenton (Hetero-EF) is limited due to its poor performance over a wide pH range. In this work, the Hetero-EF/sulfite process was constructed with FeMn@C as the catalyst to improve the degradation of pollutants under neutral pH. The removal efficiency of diclofenac (DCF) (97.8%) was significantly higher than that of Hetero-EF (15.0%) at pH 7, in which the degradation rate constant k was increased by 19.75 times. The existence and transformation process of various active species ( • OH, SO 4 •- , O 2 •- , and 1 O 2 ) in the process were verified by capture experiments and electron paramagnetic resonance (EPR) test. The possible DCF degradation pathway was also proposed. The introduction of sulfite could reduce Fe 3+ and Mn 3+ , promote the Fe(II)/Fe(III) and Mn(II)/Mn(III) cycles, strengthen the generation of active species, and thus promote the degradation of pollutants. The removal efficiency was still maintained 76.6% after five cycles. The Hetero-EF/sulfite process is a simple, feasible, and efficient method to degrade pollutants, which has a broad application prospect.
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ACS Omega
·
2025
·
IF 4.3
Tao Shen,Guodong Wu,Li Yin,Tianen Chen,JiYe Fan,Yuanhao Wang,Shifeng Wang
Developing efficient adsorbents for removal of organic pollutants and heavy metals is essential for environmental protection. In this study, a series of GO/UiO-66-(OH)2 composites were synthesized and characterized using XRD, FT-IR, and SEM, confirming enhanced thermal stability, reduced aggregation, and maintained crystallinity of UiO-66-(OH)2 due to GO incorporation. Batch adsorption experiments showed that GO increased the adsorption capacity, with GO-8/UiO-66-(OH)2 achieving 324.2 mg/g for diclofenac sodium (DCF) and 429.3 mg/g for Hg2+. DCF adsorption was primarily governed by physisorption, while Hg adsorption was chemisorptive, involving strong coordination with oxygen functional groups. Kinetic and isotherm studies revealed the suitability of the pseudo-second-order and Freundlich models, with thermodynamic analysis showing exothermic DCF adsorption and endothermic Hg2+ adsorption. The composites also exhibited high selectivity and stable regeneration, making them promising candidates for practical environmental remediation.
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CHEMOSPHERE
·
2017
·
IF 4.208
Tao Zhou,Ke Feng,Wei Xiang,Yiliang Lv,Xiaohui Wu,Juan Mao,Chang He
In this study, significant synergistic degradation of antibiotic diclofenac (DCF) was demonstrated in a novel magnetic field (MF) enhanced zero-valent iron (ZVI)/EDTA Fenton-like system. Five operational parameters, namely, initial ZVI loading, pH, EDTA dosage, DCF concentration and reaction temperature, were investigated for their effects on the DCF degradation. OH was identified as the predominant reactive oxygen species for DCF degradation in ZVI/EDTA systems whether in the presence or absence of MF. DCF molecule can be oxidized by OH, attacking via the hydroxylation and substituted dechlorination of the chlorinated aromatic ring, as well as by dehydration between the N atom and the acetoxyl. It could also be directly dechlorinated by ZVI reduction simultaneously. The reaction mechanism and promotional role of MF in the MF/ZVI/EDTA system were proposed. It is suggested that MF mainly alters the heterogeneous ZVI surface-bond reactions and accelerates the surface corrosion depending on the presence of pristine iron oxides layer, but MF does not change the homogeneous iron cycle and the Fenton-like reactions.
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