CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jinbin Lin,Yuye Hu,Junyang Xiao,Yixin Huang,Mengyun Wang,Haoyu Yang,Jing Zou,Baoling Yuan,Jun Ma
Fe(II)/peracetic acid (Fe(II)/PAA) process exhibits a great potential in abatement of micropollutants because of the fast reaction between Fe(II) and PAA. Similar to Fenton system, the slow reduction from Fe(III) to Fe(II) leads to the high dosage of Fe(II) in Fe(II)/PAA process. This study introduced 2,2′-azino-bis(3-ethylbenz- -othiazoline-6-sulfonate) (ABTS) as electron shuttle to improve the oxidation capacity of Fe(II)/PAA process by accelerating the redox cycle of Fe(III)/Fe(II). ABTS/Fe(II)/PAA process possessed high elimination efficiency of diclofenac in acidic conditions. Alcohols quenching experiments confirmed that ABTS •+ was the primary reactive species responsible for diclofenac elimination, although Fe IV O 2+ and carbon-centered radicals (R-O • ) also existed in ABTS/Fe(II)/PAA process. ABTS •+ was generated via various pathways, including the reactions of ABTS with Fe(III), Fe IV O 2+ and R-O • . ABTS was not an ideal electron shuttle because R-O • could decompose partial ABTS •+ to sulfoxides and sulfones. Two possible degradation pathways of diclofenac were proposed based on the detected transformation products. ABTS/Fe(II)/PAA process was highly-efficient for diclofenac elimination in underground water and reservoir water, while high concentration of humic acid had inhibition effect on diclofenac degradation. The present study provides a promising way to alleviate the intrinsic drawbacks of Fe(II)/PAA process and might advance its potential application in water treatment.
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 17
·6216
·
IF 4.6
Hongrui Yang,Chen Wang,Wenjuan Zhu,Pingning Jin,Fei Li,Jing Fan
A simple and efficient sample pretreatment technology is very important for the accurate determination of trace drug residues in foods to ensure food safety. Herein, we report a new carboxyl group-functionalized ionic liquid hybrid solid- phase adsorbent (PS-IL-COOH) for the highly efficient extraction and quantitative determination of diclofenac sodium (DS) residue in milk samples. It was found that the adsorption efficiency of PS-IL-COOH for the ppb level of DS was greater than 93.0%, the adsorption capacity was 934.1 mg/g, and the enrichment factor was 620.0, which surpass most of the previously reported values for DS adsorbents. The high concentration of salts did not interfere with the adsorption of DS. Importantly, the recovery of DS was above 90% after 16 adsorption–-regeneration cycles. The synergistic effect of the multiple interactions was found to be the main factor for the high efficiency of DS adsorption. The proposed method was applied to the extraction and detection of DS in milk samples, with the relative recovery ranging from 88.2 to 103.0%.Keywords:carboxyl group-functionalized ionic liquid;solid-phase extraction;diclofenac sodium;milk samples
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
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IF 11.357
Yixin Huang,Jing Zou,Jinbin Lin,Haoyu Yang,Mengyun Wang,Jiawen Li,Wei Cao,Baoling Yuan,Jun Ma
The activation of peroxydisulfate (PDS) by organic compounds has attracted increasing attention. However, some inherent drawbacks including quick activator decomposition and poor anti-interference capacity limited the application of organic compound-activated PDS. It was interestingly found that 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonate) (ABTS) could act as both activator and electron shuttle for PDS activation to enhance diclofenac (DCF) degradation over a pH range of 2.0–11.0. Multiple reactive species of ABTS•+, •OH, and SO4•– were generated in the PDS/ABTS system, while only ABTS•+ and •OH directly contributed to DCF degradation. ABTS•+, generated via the reactions of ABTS with PDS, SO4•–, and •OH, was the dominant reactive species of DCF degradation. No significant decomposition of ABTS was observed in the PDS/ABTS system, and ABTS acted as both activator and electron shuttle. Four possible degradation pathways of DCF were proposed, and the toxicity of DCF decreased after treatment with the PDS/ABTS system. The PDS/ABTS system had good anti-interference capacity to common natural water constituents. Additionally, ABTS was encapsulated into cellulose to obtain ABTS@Ce beads, and the PDS/ABTS@Ce system possessed excellent performance on DCF degradation. This study proposes a new perspective to reconsider the mechanism of activating PDS with organic compounds and highlights the considerable contribution of organic radicals on contaminant removal.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
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IF 6.361
Lihong Fan,Yuqing Lu,Li-Ye Yang,Fangfang Huang,Xiao-kun Ouyang
Hypothesis We synthesized composite microspheres from cellulose nanocrystal (CNC), polyvinyl alcohol (PVA), and sodium alginate (SA), which were modified with polyethyleneimine (PEI) to introduce a high density of active amino sites onto the surface via the Schiff base reaction. We hypothesized that these (SA/CNC/PVA)@PEI microspheres would have a high adsorption capacity for aqueous diclofenac sodium (DS). Experiments The PEI-modified composite microspheres were characterized and assessed and optimized for aqueous DS adsorption. In addition, the morphology and synthesis mechanism of the adsorbent were studied. Findings The adsorption process showed a good fit with the pseudo-second-order kinetic model (i.e., the process is driven by a chemical adsorption mechanism) and Langmuir adsorption isotherm model (i.e., adsorption follows a single-layer process). Under the optimum experimental conditions (pH: 4.5, adsorption time: 50 min, temperature: 303 K), the maximum adsorption capacity was 418.4104 mg/g, which was relatively high compared to other reported adsorbents. Importantly, after five adsorption–desorption cycles, (SA/CNC/PVA)@PEI showed only a slight loss in adsorption capacity. Compared with other reported adsorbents, the core–shell composite has a good DS adsorptive capacity and high recyclability.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Zhou Li,Jia Zeng,Min Wang,Die Gao,Deng Li,Yingxi Zhu,Jiahao Lin,Zhiyu Chen,Famin Ke,Lixian Li,Dandan Wang
Diclofenac potassium (DCF-K) is a widely used nonsteroidal anti-inflammatory drug with enhanced therapeutic effects mediated by its bioactive metabolites, particularly 4′-hydroxydiclofenac (4′-OH-DCF) and 5-hydroxydiclofenac (5-OH-DCF). However, the accurate detection of DCF-K and its metabolites in complex biological matrices remains challenging due to trace concentrations and matrix interference. To address this challenge, a chitosan-bentonite molecularly imprinted polymer (CB-MIP) was developed using a dual-role strategy, where chitosan-bentonite (CB) serves as both substrate and functional monomer, combined with a hierarchical functional monomer system (acrylamide as an auxiliary monomer) to enhance binding affinity and selectivity for the specific capture of DCF-K and its metabolites. Comprehensive characterization confirmed the successful synthesis of CB-MIP, revealing improved stability, hydrophilicity, and a mesoporous structure. CB-MIP exhibited good adsorption capacity for DCF-K (17.2× higher than CB), with Langmuir isotherm and pseudo-second-order kinetics indicating monolayer chemisorption. Selectivity studies demonstrated good recognition capability for DCF-K, achieving a selectivity factor up to 77.3 against structural analogs and co-administered drugs. Furthermore, cluster analysis revealed the CB-MIP sensitivity to DCF-K concentration variations as low as 0.3 μg·mL −1 in complex matrices. Mechanistic studies identified electrostatic and hydrogen bonding interactions as the primary binding forces, validated by electrostatic potential simulations, hydrogen-bond modeling, and spectroscopic analyses. Practical application in mouse plasma and liver samples confirmed efficient enrichment and detection of DCF-K and metabolites (4′-OH-DCF, 5-OH-DCF, diclofenac acyl glucuronide) using CB-MIP coupled with HPLC/UPLC-MS/MS, achieving high sensitivity (limit of detection: 0.231 μg·mL −1 in liver) and reproducibility (relative standard deviation: 1.22 %–5.81 %). This work establishes CB-MIP as a robust pretreatment material for targeted drug/metabolite analysis in complex biological systems.
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高影响因子
Polymers
·
2020
·Vol. 12
·期 1
·72
·
IF 3.426
Qiang Sun,Huaili Zheng,Xuebin Hu,Jun Li,Rui Zhao,Chun Zhao,Wei Ding
In this study, a novel system was set up by preparing a magnetic flocculant combining with ultraviolet/H2O2to realize the rapid enrichment and degradation of diclofenac sodium (DCFS). For the magnetic flocculant, template anion polyacrylamide (TAPAM) with anion micro-block structure was prepared. Thereafter, polydopamine was used to modify TAPAM, Fe3O4nanoparticles was grafted to the modified TAPAM by chelation, named template anion polyacrylamide-polydopamine-Fe3O4(TAPAM-PDA-Fe3O4). Furthermore, the TAPAM-PDA-Fe3O4preparation protocol was optimized by the response surface method (RSM). In the DCFS enrichment section, the rapid separation of flocs from water was realized by an external magnetic field and it indicated that the π–π stacking effect was dominant in neutral/alkaline condition, whereas charge neutralization was favored in acidic conditions. Meanwhile, a DCFS enrichment kinetic curve was much fitted by the pseudo-second-order kinetic model and DCFS enrichment isothermal curve was close to the Freundlich isothermal model, indicating the dependence of DCFS quantity enriched by TAPAM-PDA-Fe3O4and a multilayer heterogeneous enrichment process. The degradation experiment confirmed that DCFS was effectively degraded by ultraviolet/H2O2/TAPAM-PDA-Fe3O4and the maximum value of DCFS degradation efficiency reached 98.1%. Furthermore, the regeneration experiment showed that the enrichment and degradation efficiency of DCFS could maintain a relatively high level in the initial three recycles.Keywords:diclofenac sodium;π–π stacking;charge neutralization;enrichment;degradation
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shiling Liu,Jingjing Hui,Huandi Li,Yijun Li,Xiwen He,Langxing Chen,Yukui Zhang
In recent years, ion covalent organic frameworks (iCOFs) have shown excellent adsorption performance in the removal of non-steroidal anti-inflammatory drugs (NSAIDs), but powdered iCOFs are faced with problems in separation and recovering from solution and are prone to environmental pollution. In this work, polydopamine (PDA) was used as the mediated coating, Fe 3 O 4 as the magnetic nucleus, and iCOFs consisting of benzene-1,3,5-triscarbaldehyde (BT) and 1,3-diaminoguanidine hydrochloride (DG Cl ) as organic ligands were in-situ grown on the surface of the PDA coating by Schiff base reaction, resulting in a magnetic nanocomposite (Fe 3 O 4 @PDA@BT-DG Cl ) with a coral-like structure. The adsorption kinetics and adsorption isotherms showed that the adsorption behavior of diclofenac sodium (DS) on Fe 3 O 4 @PDA@BT-DG Cl followed the pseudo-second-order kinetic model and Langmuir model, and the maximum adsorption capacity could reach up to 420.17 mg g −1 (25 ℃, pH 5). The adsorption of DS on Fe 3 O 4 @PDA@BT-DG Cl was dominated by electrostatic interactions, along with hydrogen bonding, π-π interactions, and ion exchange, according to the analysis of the adsorption mechanism. The Fe 3 O 4 @PDA@BT-DG Cl consistently maintained high adsorption efficiency after six adsorption–desorption cycles, making it an efficient adsorbent for the removal of NSAIDs in complex water environments.
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高影响因子
Reaction Chemistry & Engineering
·
2021
·Vol. 6
·期 12
·2411-2424
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IF 4.239
Shuaiqi Ning,Shuai Mao,Chun Liu,Mingzhu Xia,Fengyun Wang
In this paper, some perovskite catalysts LaFeO3 (LFO) were prepared by using the efficient chelating properties of sodium diethylene triamine pentamethylene phosphonate (DTPMP-2Na) toward metal ions, and the best catalyst LFO-0.1 was selected by using diclofenac sodium as the target pollutant. Then, the influence of different factors (PMS dosage, catalyst dosage, substrate concentration and anion) on the degradation of DCF in a LFO-0.1/PMS system was studied. The catalyst was characterized, and the reaction mechanism of diclofenac (DCF) in the LFO-0.1/PMS system was analyzed. It was concluded that hydroxyl radicals, sulfate radicals and singlet oxygen were produced in the LFO-0.1/PMS system. In the reaction system, singlet oxygen is considered to be the main factor for DCF degradation in this system, and the generation of sulfate radicals is mainly attributed to oxygen vacancies and the electron transfer between Fe3+ and Fe2+. Through the centrifugal recovery of the catalyst to explore its stability, the conclusion is that LFO-0.1 is a stable catalyst. Finally, 15 kinds of oxidation intermediates and products were identified, and the possible degradation pathways of DCF were analyzed, including decarboxylation, dechlorination, C–N cleavage, hydroxylation, ring-closure and ring-opening.
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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2018
·
IF 3.849
Weirui Chen,Zulin Zhang,Xukai Li,Dan Wu,Ying Xue,Laisheng Li
Fe-Cu-MCM-41/O 3 was first used as an alternative to O 3 to control disinfection by-products generation from chlorinated-disinfection of Br-containing Diclofenac. Accompanying with decrease of TOC , THMs and HAAs had an initial increase, reaching the highest at 30 min, then gradually decreased. Coupling Fe-Cu-MCM-41 with O 3 successfully enhanced TOC removal and inhibited bromate, THMs and HAAs formation in post-chlorination when compared with those in ozonation . Four kinds of THMs and six kinds of HAAs were detected. CHCl 3 was main Cl-THMs and CHBrCl 2 was main Br-THMs. CHCl 2 COOH was the dominant Cl-HAAs and CHClBrCOOH was main Br-HAAs. A converse Br-THMs order was observed in O 3 and Fe-Cu-MCM-41/O 3 pre-treatment. Fe-Cu-MCM-41 decreased ozone exposure, reducing the direct reaction of O 3 with Br − to form bromate. More DBPs precursors in Fe-Cu-MCM-41/O 3 were removed by ·OH. H 2 O 2 , which generated during pre-treatment process, reduced HBrO/BrO − to Br − , inhibiting both its reaction with Br-DBPs precursors and bromate formation. The pre-treatment process changed intermediates’ properties and hydrophilic DOM was the dominant component. Hydrophobic acids and transphilic DOM were the main chlorine consuming intermediates and had major contribution to DBPs formation. Fulvic-like intermediates was suggested as precursors of Br-DBPs. Fe-Cu-MCM-41/O 3 were suggested as a good alternative to O 3 pretreatment.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Haihua Xu,Sidi Zhu,Mingzhu Xia,Fengyun Wang
The efficient removal of Diclofenac sodium (DCF), a nonsteroidal anti-inflammatory drug, has attracted more and more attention. In this work, ternary core-shell CS@PANI@LDH composite was synthesized via the in-situ growth of Mg/Al layered double hydroxide plates onto polyaniline-wrapped carbon sphere and applied for DCF removal. Various influence factors like concentration, pH, time, temperature, and background electrolytes were systematically investigated. The maximum adsorption capacity was 618.16 mg/g. Besides, after 5 regeneration cycles, CS@PANI@LDH still retained high adsorption capacity. The adsorption mechanism was investigated by Fourier transformed infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS) characterization analyses. Simultaneously, the Multiwfn program combined the Chimera program was applied to calculate and visualize the localized orbit locator (LOL) of π electrons in DCF − molecule, which explored the π electronic structure and conjugation characteristics of DCF − molecule. Moreover, the Independent Gradient Model (IGM) analysis based on pro-molecular density revealed the interaction sites and interaction strength between DCF and LDH. The adsorption mechanism could be explained through electrostatic interaction and hydrogen bonding between LDH and DCF, π-π interaction between DCF and PANI. It was the synergistic effects of different interactions that improved the adsorption of DCF by CS@PANI@LDH composite.
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高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Qing Huang,Xiaokun Li,Suxiang Feng,Wenfeng Zhuge,Jinyun Peng,Xiaoting Li
Ag nanoparticles functionalized with poly-acid chrome blue K and graphene (Ag-poly-ACBK@Gr) were successfully fabricated on the surface of a glassy carbon electrode using layer-by-layer electropolymerization. The surface structure of the synthesized modified glassy carbon electrode was characterized by scanning electron microscopy. The electrochemical behaviours of diclofenac sodium (DS) at the Ag-poly-ACBK@Gr-modified electrode were investigated by cyclic voltammetry and differential pulse voltammetry. It was found that the prepared sensor exhibited a cathodic peak at 0.78 V with higher peak current response compared to the related modified electrodes. Under optimal conditions, the sensor for the determination of DS exhibits a good linear relationship between the peak current and DS concentration in the range from 0.1 to 40 μM, and the equation is Ip (μA) = 7.23 × 10 3 c (μM) + 3.46 × 10 -2 (R = 0.9955) with the estimated limit of detection of 34.2 nM (S/N = 3). The Ag-poly-ACBK@Gr-modified glassy carbon electrode with high sensitivity and excellent stability and selectivity was successfully applied to detect DS in real drugs and human urine at the recoveries ranging from 99.60 to 101.84%.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
·
IF 3.359
Junfeng Zhao,Yiqing Liu,Qun Wang,Yongsheng Fu,Xiaohui Lu,Xiaofeng Bai
In this study, the effect of phosphate, Fe(III), Fe(II), and reductive substances (i.e., Mn 2+ and SO 3 2− ) on diclofenac (DCF) oxidation and its degradation mechanism by Ferrate (Fe(VI)) were investigated. The removal rate of DCF in reaction solution at pH 9.0 adjusted by NaOH (67.36%) was higher than that by phosphate buffer (14.87%) because of the complexation of phosphate with Fe(III) and/or Fe(II) restraining the self-catalysis of Fe(VI). Fe(III) or Fe(II) could significantly catalyze Fe(VI) to generate more intermediates (i.e., Fe(V) and Fe(IV)), whose oxidation capacity was magnitude stronger than that of Fe(VI), leading to the improvement of DCF degradation, besides, the presence of reductive substances, e.g., Mn 2+ and SO 3 2− , could also increase the self-catalysis of Fe(VI), enhancing the removal of DCF, which will be further verified in follow-up studies. Seven oxidation products (OPs) were detected using a quadrupole-time of flight-mass spectrometer coupled with an ultra performance liquid chromatograph (LC-QTOF/MS). Based on these identified OPs, the potential degradation mechanism of DCF by Fe(VI) was proposed showing six reaction pathways, including hydroxylation, decarboxylation, C N bond cleavage, dehydrogenation, formylation, and dechlorination-hydroxylation. This study suggests that Fe(VI) can effectively oxidize and degrade DCF.
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