Nanomaterials
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2022
·Vol. 12
·期 16
·2834
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IF 5.719
Yun He,Hongjie Gao,Jiankang Liu
Diclofenac is a non-steroidal, anti-inflammatory drug and is clinically used for the treatment of osteoarthritis, non-articular rheumatism, etc. This research aimed to demonstrate the creation of an upgraded photoelectrochemical (PEC) aptamer sensor for detecting diclofenac (DCF) with high sensitivity. In this work, photoactive materials and bio-identification components served as visible-light-active CuS/MoS2/Bi2WO6heterostructures and aptamers, respectively. CuS and MoS2/Bi2WO6were combined to improve photocurrent responsiveness, which helped the structure of PEC aptasensors. Additionally, the one-pot synthesis of CuS/MoS2/Bi2WO6was ecologically beneficial. With these optimizations, the photocurrent response of aptamer/CS/CuS/MoS2/Bi2WO6exhibited linearity between 0.1 and 500 nM DCF. The detection limit was 0.03 nM (S/N = 3). These results suggest that the PEC sensing technique might produce an ultra-sensitive sensor with high selectivity and stability for DCF detection.Keywords:photoelectrochemical;CuS/MoS2/Bi2WO6;diclofenac (DFC);heterostructure;aptasensors
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Xianjing Zhou,Feng Chen,Haipeng Lu,Lingli Kong,Siyu Zhang,Wei Zhang,Jingjing Nie,Binyang Du,Xinping Wang
In this study, we designed and synthesized hybrid microgels with a positively charged cross-linking network and embedded gold nanoparticles. The hybrid microgels presented reversible thermosensitive behavior and the volume transition temperature of ∼37 °C, which was close to body temperature. These microgels were successfully applied as vectors to simultaneously deliver hydrophobic anticancer drug, doxorubicin, and anionic anti-inflammatory drug, diclofenac sodium. In the tumor microenvironment of low pH, high temperature, reduction condition, and the presence of ions, both drugs could controllably release from the microgels. Such microgels might be a promising platform for further development as an effective strategy for combination therapy.
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CHEMOSPHERE
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2018
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IF 4.427
Xukai Li,Weirui Chen,Yiming Tang,Laisheng Li
Fe-MCM-48 catalyst with a three-dimensional cubic pore structure was directly synthesized via a hydrothermal method, and the mineralization efficiency of diclofenac (DCF) in the catalytic ozonation process (Fe-MCM-48/O 3 ) was assessed. X-ray diffraction (XRD), N 2 adsorption desorption, transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) characterizations revealed that Fe existed in the framework of MCM-48, and Fe-MCM-48 possessed a large surface area and a highly ordered cubic mesoporous structure, which could accelerate reactants and products diffusion. Regarding mineralization efficiency, the addition of Fe-MCM-48 significantly improved total organic carbon (TOC) removal, and approximately 49.9% TOC were removed through the Fe-MCM-48/O 3 process at 60 min, which was 2.0 times higher than that in single ozonation. Due to this catalyst's superior structure, Fe-MCM-48 showed the better catalytic activity compared with Fe-MCM-41 and Fe loaded MCM-48 (Fe/MCM-48, Fe existed on the surface of MCM-48). DCF removal in the Fe-MCM-48/O 3 process was primarily based on ozone direct oxidation. The improvement of mineralization efficiency was attributed to the function of generated hydroxyl radicals (•OH), which indicated that the presence of Fe-MCM-48 accelerated ozone decomposition . Moreover, the negatively charged surface of Fe-MCM-48 and the proper pH value of the DCF solution played an essential role in OH generation.
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JOURNAL OF MOLECULAR STRUCTURE
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2021
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IF 3.196
Wen-Quan Feng,Ling-Yang Wang,Jie Gao,Ming-Yu Zhao,Yan-Tuan Li,Zhi-Yong Wu,Cui-Wei Yan
To improve the physicochemical properties of diclofenac (DFA) and exert its potential anti-tumor effect in combined pharmacotherapy of metformin (MET), a new drug-drug molecular salt of DFA and MET (DFA-MET) is formed and characterized. The single-crystal X-ray diffraction analysis shows that DFA-MET is a three-dimensional (3D) supramolecular structure constructed by different hydrogen-bonding interactions between DFA and MET with 1:1 stoichiometry by proton transfer reaction. In addition, Hirshfeld Surface analysis shows that both the hydrogen-bonding interactions and the Vander Waals maintain the 3D supramolecular structure of DFA-MET together. Compared with pure DFA and pure diclofenac sodium (NaDFA), the dissolving behavior and permeability of DFA-MET by forming drug-drug molecular salt in physiological pH environments are enhanced remarkably.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Qian Zhang,Hao-Zhe Li,Bing Li,Sha Li
The efficient removal of emerging anionic organic pollutants, particularly pharmaceuticals and herbicides such as sodium diclofenac (DCF-Na) and sodium 2,4-dichlorophenoxyacetate (2,4- D -Na), from aqueous environments remains a significant challenge. Although hydrochar is a sustainable and low-cost adsorbent, its intrinsic negative surface limits its affinity for anionic contaminants. To overcome this, a novel mesoporous poly(imidazolium)-grafted hydrochar (PIHC) was synthesized via a one-pot in situ quaternization polymerization by directly grafting 1,3,5-tris(1H-imidazol-1-yl)benzene and 1,3,5-tris(bromomethyl)benzene onto bamboo hydrochar. The impact of aqueous pH, adsorbing temperature, ionic strength and contact time on the removal of DCF-Na and 2,4- D -Na by PIHC was systematically investigated. The resulting PIHC exhibited rapid and efficient adsorption, removing 52 % of DCF-Na (C 0 = 400 mg·L −1 ) and 88 % of 2,4- D -Na (C 0 = 100 mg·L −1 ) within 5 min. The adsorption kinetic and isotherm data fitted well with the pseudo-second-order kinetic model and the Langmuir model, indicating that the adsorption was dominated by monolayer chemical adsorption. Thermodynamic test uncovered a spontaneous and endothermic adsorption, with the spontaneity mainly driven by entropy. The high performance is attributed to the synergistic effects of the mesoporous structure and high positive charge density, enabling multiple mechanisms including electrostatic attraction, ion exchange, and π-π interactions. This work provides a versatile molecular design strategy for developing high-performance, imidazolium-grafted hydrochar for pharmaceutical and herbicide remediation.
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Journal of Cleaner Production
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2022
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IF 11.072
Bin Zhang,Meng Mei,Kaiwei Li,Jingxin Liu,Teng Wang,Si Chen,Jinping Li
Magnetic biochar adsorbents often suffer from the uneven distribution and shedding problems of nanoparticles . In this study, a one-pot sol-gel pyrolysis method was proposed to synthesize a MnFe 2 O 4 functionalized magnetic sawdust-based biochar (MnFe 2 O 4 @SBC) for efficient removal of diclofenac sodium (DCF). The MnFe 2 O 4 @SBC was characterized by XRD , Raman, VSM, TG-DSC, SEM, TEM, BET, FTIR and XPS . The results demonstrated that the combination of sol-gel and sawdust effectively led to a homogeneous distribution of MnFe 2 O 4 on biochar and the MnFe 2 O 4 @SBC possessed a much richer pore structure and functional groups than the original biochar. A systematic comparison of MnFe 2 O 4 @SBC with commercial activated carbon (CAC) was conducted by analyzing the effects of initial pH, adsorbent dosage, coexisting ions, contact time and temperature on their adsorption performance. Based on the adsorption isotherm study, the maximum adsorption capacity of MnFe 2 O 4 @SBC was predicted to be 352.17 mg/g, which was almost 3.5 times that of CAC. Selectivity adsorption study and real water-based removal experiment further demonstrated the satisfactory adsorption selectivity and applicability of MnFe 2 O 4 @SBC for DCF. This study reveals that the one-pot sol-gel pyrolysis is a promising method for synthesizing excellent magnetic biochar adsorbents.
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LANGMUIR
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2023
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IF 3.9
Siqi Liang,Kangkang Wang,Kefu Wang,Tao Wang,Changyan Guo,Wei Wang,Jide Wang
To unveil the intricacies surrounding the interaction between microplastics (MPs) and pollutants, diligent investigation is warranted to mitigate the environmental perils they pose. This exposition delves into the sorption behavior and mechanism of diclofenac sodium (DCF), a contaminant, upon two distinct materials: polystyrene (PS) and poly(butylene adipate-co-terephthalate) (PBAT). Experimental adsorption endeavors solidify the observation that the adsorption capacity of DCF onto the designated MPs amounts to Q(PBAT) = 9.26 mg g–1 and Q(PS) = 9.03 mg g–1, respectively. An exploration of the factors governing these discrepant adsorption phenomena elucidates the influence of MPs and DCF properties, environmental factors, as well as surfactants. Fitting procedures underscore the suitability of the pseudo-second-order kinetic and Freundlich models in capturing the intricacies of the DCF adsorption process onto MPs, corroborating the notion that the mentioned process is characterized by non-homogeneous chemisorption. Moreover, this inquiry unveils that the primary adsorption mechanisms of DCF upon MPs encompass electrostatic interaction, hydrogen bonding, and halo hydrogen bonding. An additional investigation concerns the impact of commonly encountered surfactants in aqueous environments on the adsorption of DCF onto MPs. The presence of surfactants elicits modifications in the surface charge properties of MPs, consequently influencing their adsorption efficacy vis-à-vis DCF.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Liuyang He,Lixin Lv,Suresh C. Pillai,Hailong Wang,Jianming Xue,Yongfei Ma,Yanli Liu,Yulin Chen,Li Wu,Zulin Zhang,Lie Yang
Iron/copper bimetallic nanoparticles based sludge biochar (Fe/Cu-SBC) was prepared by using a modified co-precipitation route. The Fe/Cu-SBC system prepared was subsequently applied to activate periodate (IO 4 − ) to degrade diclofenac sodium (DCF) by using UV light at room temperature (25 °C). The physicochemical properties of both SBC and Fe/Cu-SBC such as morphology, physical properties, crystal structures and functional groups were examined. The type and number of surface functional groups were found to be increased and the catalytic performance was improved by the modification of Fe/Cu bimetallic nanoparticles. The influence of various parameters to evaluate the catalytic efficiency such as periodate (PI) concentration, dosage of catalysts, UV power, initial pH and coexisting anions were investigated. Under the optimized conditions (pH 6.9, UV-power 60 W, PI concentration of 5 mM and 0.1 g Fe/Cu-SBC), it was observed that 99.7% of DCF was degraded with a pseudo-first-order kinetics reaction constant 9.39 × 10 −2 min −1 . The radical scavenging experiments showed that IO 3 radicals were the predominantly reactive oxidants in the Fe/Cu-SBC/UV system. Therefore, this investigation provides a feasible alternative for the degradation of PPCPs in wastewater.
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WATER RESEARCH
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2021
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IF 11.236
Jinbin Lin,Jing Zou,Hengyu Cai,Yixin Huang,Jiawen Li,Junyang Xiao,Baoling Yuan,Jun Ma
In this study, a commonly used reducing agent, hydroxylamine (HA), was introduced into Fe(II)/PAA process to improve its oxidation capacity. The HA/Fe(II)/PAA process possessed high oxidation performance for diclofenac degradation even with trace Fe(II) dosage (i.e., 1 μM) at pH of 3.0 to 6.0. Based on electron paramagnetic resonance technology, methyl phenyl sulfoxide (PMSO)-based probe experiments and alcohol quenching experiments, Fe IV O 2+ and carbon-centered radicals (R-O • ) were considered as the primary reactive species responsible for diclofenac elimination. HA accelerated the redox cycle of Fe(III)/Fe(II) and itself was gradually decomposed to N 2 , N 2 O, NO 2 − and NO 3 − , and the environmentally friendly gas of N 2 was considered as the major decomposition product of HA. Four possible degradation pathways of diclofenac were proposed based on seven detected intermediate products. Both elevated dosages of Fe(II) and PAA promoted diclofenac removal. Cl − , HCO 3 − and SO 4 2− had negligible impacts on diclofenac degradation, while humic acid exhibited an inhibitory effect. The oxidation capacity of HA/Fe(II)/PAA process in natural water matrices and its application to degrade various micropollutants were also investigated. This study proposed a promising strategy for improving the Fe(II)/PAA process and highlighted its potential application in water treatment.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Yixin Huang,Jinbin Lin,Jing Zou,Jiaxin Xu,Mengyun Wang,Huahua Cai,Baoling Yuan,Jun Ma
Horseradish peroxidase (HRP)-catalyzed hydrogen peroxide (H 2 O 2 ) oxidation could degrade a variety of organic pollutants, but the intrinsic drawback of slow degradation rate limited its widespread application. In this study, 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) was introduced into HRP/H 2 O 2 system as an electron shuttle to enhance diclofenac degradation under neutral pH conditions. The green-colored ABTS radical (ABTS •+ ), generated by the oxidation of ABTS with HRP-catalyzed H 2 O 2 oxidation, was proved to be the main reactive species for the rapid degradation of diclofenac in HRP/H 2 O 2 /ABTS system. There was no destruction of ABTS/ABTS •+ in HRP/H 2 O 2 /ABTS system, and ABTS was verified as an ideal electron shuttle. The reaction conditions including solution pH (4.5–10.5), HRP concentration (0–8 units mL −1 ) and H 2 O 2 concentration (0–500 μM) would impact the formation of ABTS •+ , and affect the degradation of diclofenac in HRP/H 2 O 2 /ABTS system. Moreover, compared with Fenton and hydroxylamine/Fenton systems, HRP/H 2 O 2 /ABTS system had better diclofenac degradation efficiency, higher H 2 O 2 utilization efficiency and stronger anti-interference capacity in actual waters. Overall, the present study provided a meaningful and promising way to enhance the degradation of organic pollutants in water with HRP-catalyzed H 2 O 2 oxidation.
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ACS Applied Bio Materials
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2019
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IF 0
Yan Ma,Junhong Zhou,Zhaohua Miao,Haisheng Qian,Zhengbao Zha
Cancer cells with up-regulated intracellular heat shock proteins (HSPs) expression under adverse heat environment during photothermal therapy (PTT) always resulted in inefficient oncotherapy. As the expression of HSPs is an energy-dependent manner, inhibiting the aerobic glycolysis pathway to realize tumor starvation and therefore consequently reducing the production of intratumoral adenosine 5′-triphosphate (ATP) would offer an efficient way for sensitizing cancer cells to PTT. DLM@PPy NPs, a polypyrrole (PPy)-based platform complexing with dl-menthol (DLM), was well-designed and successfully developed here as a near-infrared (NIR) light and thermo responsive drug delivery system. Benefiting from the volatile property of DLM and high photothermal conversion ability of PPy, the as-prepared DLM@PPy NPs could continuously generate bubbles under NIR light illumination, which is good for precisely controlling the release of encapsulated drug and monitoring the whole therapeutic process by ultrasound imaging. By encapsulating diclofenac (DC, an inhibitor of glucose transporter 1 to realizing tumor starvation) to form DC/DLM@PPy NPs, on-demand DC release could be easily achieved by selectively turning on/off the NIR light irradiation. After releasing DC in tumor lesion to reduce the generation of intratumoral ATP, a significant intensified cell-killing efficiency of PTT was observed. Thus, our study has demonstrated the good potential of DLM/PPy NPs as a stimuli-responsive DC delivery system for intensified PTT through inhibiting the aerobic glycolysis of cancer cells.
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CARBOHYDRATE POLYMERS
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2019
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IF 6.044
Yuqing Lu,Lihong Fan,Li-Ye Yang,Fangfang Huang,Xiao-kun Ouyang
Residual diclofenac sodium (DS) in water is a potential hazard. The electrostatic attraction between amino group of adsorbents and carboxyl group of DS under acidic conditions can effectively remove DS from water. Herein, a novel core–shell adsorbent of poly(vinyl alcohol)/chitosan/amino-grafted silica@polyethylenimine (PVA/CS/SAP@PEI) gel bead was prepared to efficiently uptake DS from wastewater. In this study, the gel bead was characterized using FTIR, XPS, SEM, EDS, and 13 C NMR. The experimental data shows that there is a strong correlation between adsorption capacity. The adsorption data fitted well with the Freundlich isotherm model and the pseudo-second-order model. The results of thermodynamics show that the adsorption process is spontaneous, endothermic, and increases entropy. The maximum adsorption capacity for DS was calculated as 493.81 mg/g at pH 5 (308 K). The adsorbent still exhibited excellent adsorption capacity after recycling five times, showing it has excellent potential for practical applications.
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