JOURNAL OF SOLID STATE CHEMISTRY
·
2025
·
IF 3.5
Shaopeng Zhang,Jie Ding,Dayong Tian,Jing Wang,Ruiqin Kang,Jiaohui Xia,Shengbo Yang,Minghua Lu
The effective removal of diclofenac sodium (DCF) has become an important topic in waste management because of its poor efficiency in wastewater treatment. In this study, covalent organic polymer (COPs) were modified with vinylbenzyl trimethylammonium chloride (VTC), an organic compound containing abundant aromatic rings and quaternary ammonium groups. The structure of the resulting adsorbent (VTC-COPs) was investigated via FTIR, XRD, TGA, SEM, BET, and XPS. The modified VTC-COPs exhibited a mesopore structure with a pore size of 27.9 nm and a specific surface area of 38.5 m 2 /g. The DCF removal performance of VTC-COPs in aqueous solutions was evaluated by a batch adsorption experiment. At pH 6, the saturated adsorption capacity of VTC-COPs reached 458 mg/g, whereas that of the original C C-COPs was 346 mg/g. The results show that the Langmuir adsorption isotherm and pseudo-second-order kinetic models can effectively describe the equilibrium adsorption process. According to the Langmuir model, the maximum adsorption capacity of the adsorbent VTC-COPs at 298 K was 616 mg/g. The negative ΔH and ΔG values obtained through thermodynamic parameters confirmed that the DCF adsorption of VTC-COPs was a spontaneous exothermic process. Coexisting ions influenced adsorption in the following order: PO 4 3− > SO 4 2− > CO 3 2− > NO 3 − > Cl − . The desorption experiment shows that DCF desorption can recover the material in a 0.1 mol/L NaOH solution. After 10 sorption-desorption cycles, the performance loss of VTC-COPs was only 5 %. The post-adsorption FTIR, BET, SEM, and XPS analysis results show that the nitrogen functional groups and aromatic rings of VTC-COPs interact with DCF. The adsorption mechanism is primarily based on electrostatic interaction, π–π interaction, and pore filling. According to these results, VTC-COPs can be considered a viable adsorbent for removing DCF from wastewater.
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高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Mingi Ko,Jin-Hyuk Choi,Taesoon Jang,Soyeong Yoon,Jae-Woo Choi,Jeong-Ann Park
The interconnected macroporous graphene oxide-chitosan (GO-CS) sponge endowed the ability to simultaneously remove diclofenac (DCF), triclosan (TCS), and polystyren microplastics (PS MPs). Compared to the adsorption capacity for a single pollutant, the adsorption capacity for TCS and PS MPs was slightly decreased, indicating the partial competition of adsorption sites; however, the major adsorption sites for each pollutant differed. Fourier transform infrared and X-ray photoelectron spectroscopy analyses revealed that the adsorption of the pollutants onto the GO-CS sponge was influenced by electrostatic interactions, hydrogen bonding, and π-π interactions. The GO-CS sponge effectively removed DCF, TCS, and PS MPs even in real water samples. While DCF removal decreased in effluent and river water due to elevated pH and ion competition, TCS and PS MPs removal remained stable, driven by hydrophobic and π-π interactions. Under the flow-through condition, the highest adsorption capacities for DCF (20.49 mg/g), TCF (18.15 mg/g), and PS MPs (6.43 mg/g) were observed at the lowest flow rate (1.52 mL/min). All the breakthrough curves for the adsorption of the pollutants were described well by the Clark model, indicating their favorable and multilayer adsorption. Further, the sponge maintained its morphology and adsorption capacity (> 90.4 %) after three cycles of adsorption/desorption. Additionally, the GO-CS sponge exerted no toxicity on Daphnia magna (48 h of exposure) and no growth inhibition effect on Pseudokirchneriella subcapitata (72 h of exposure). The sponge lost 54.28 % of its total weight after being buried in the soil for 35 days, verifying its biodegradability.
研究领域:
环境科学
·
材料科学
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高影响因子
JOURNAL OF INCLUSION PHENOMENA AND MACROCYCLIC CHEMISTRY
·
2019
·Vol. 94
·期 1
·85-94
·
IF 1.429
Li Shuhan,Tang Yue,Zhang Xinru,Dou Yushun,Shen Xiangchun
This research is to study on preparation and characterization of diclofenac sodium β-cyclodextrin (DS-β-CD) inclusion complex eye drops in order to improve the solubility of diclofenac sodium (DS) and reduce the irritation of DS eye drops in the market. First, DS-β-CD inclusion complex was prepared by co-precipitation method and then mixed with excipients to prepare inclusion complex eye drops. Finally, instruments were used to determine the basic properties of eye drops and animal experiments were used to investigate the irritation of the DS-β-CD inclusion complex eye drops. The drug content, the encapsulation efficiency and the yield of DS-β-CD inclusion complex were respectively 17.11, 84.20 and 60.00%. And the DS-β-CD inclusion complex was identified by FTIR, DSC, XRD and 1 HNMR. The solubility of the inclusion complex was 20 times more than DS. The pH value, the osmotic pressure, the viscosity and the drug content of the eye drops were respectively 7.20, 298 mosmol/kg, 4.88 mPa s and 97.98%. In brief, DS-β-CD inclusion complex eye drops had stable properties, high solubility and the test items met the requirements. The eye drops were almost non-irritating, significantly reducing the irritation of the original prescription (P < 0.01).
研究领域:
药剂学
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药物化学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Dalin Hu,Haoyu huang,Ran Jiang,Nan Wang,Hongping Xu,Yang-Guang Wang,Xiao-kun Ouyang
Residual diclofenac sodium (DS) in the environment is harmful to human health. A promising method for DS removal is the use of adsorbents functionalized with amino groups that can form an ionic bond with the carboxyl group of DS at a suitable pH. In this work, a novel composite adsorbent composed of cellulose nanocrystals (CNC) and chitosan (CS) has been synthesized and functionalized by ethylenediamine (ED) in both layers. Characterization methods, including scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, Fourier-transform infrared spectrometry, and X-ray photoelectron spectroscopy, were used to confirm the morphology and synthetic mechanism of the double- amino-functionalized adsorbent. Based on the optimization of adsorption conditions and modeling of the adsorption mechanism, the DS adsorption process on CNC-ED@CS-ED involves chemical adsorption, and the maximum adsorption capacity obtained from the Langmuir model is 444.44 mg/g. CNC-ED@CS-ED exhibits good adsorption capacity and high sustainability; thus, it is a promising composite material for the removal of DS from wastewater.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Shanshan Liu,Xu Zhao,Huabin Zeng,Yanbin Wang,Meng Qiao,Wei Guan
In this work, persulfate (S 2 O 8 2− , PS) was introduced to the photoelectrocatalytic (PEC) system, which consisted of a γ-Bi 2 MoO 6 photoanode and a copper foil cathode (Bi 2 MoO 6 /Cu/PEC/PS system). Significant enhancement of diclofenac sodium (DCF) degradation efficiency was observed in this system under visible light irradiation. At an applied bias of 1.5 V and initial solution pH of 5.62, the removal efficiency of DCF with an initial concentration of 10 mg/L was increased from 19.4% in the PEC process to 86.3% in the PEC process with 10 mM PS addition. The pseudo-first-order kinetic rate constant of DCF degradation was increased from 0.1112 h −1 to 1.0498 h −1 . Active free radicals involving SO 4 − and HO were produced in this process, which were confirmed by electron spin resonance analysis. Furthermore, the surface variation of copper foil cathode was characterized by FE-SEM, GI-XRD, XPS and in situ Raman spectroscopy. It was demonstrated that Cu 2 O formed on the surface in the reaction process with the S 2 O 8 2− addition, which was further confirmed by the photoelectrochemical analysis of the cathode. The surface Cu(0)–Cu(I)–Cu(II)–Cu(0) redox cycle of cathode was proposed, which was responsible for the persulfate activation, leading to the generation of free radicals. This work may provide a new perspective on the combined utilization of different technologies for catalytic contaminant removal.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 27
·41776-41787
·
IF 5.19
Huang Jialei,He Jingjing,Xu Keneng,Xiang Yali,Luo Yan
Owing to high treatment efficiency under neutral condition and no extra energy required, copper-mediated activation of persulfate (PS) has been widely used for the degradation of refractory organic pollutants in water. The dispersion stability of copper nanoparticle in water, however, remains a great challenge. Meanwhile, chemical oxidative modification of graphene oxide (GO) can improve the dispersion stability of GO in water. In this paper, cuprous oxide (Cu 2 O) was deposited on the surface of GO. GO/Cu 2 O nano-composites with different mass ratios, i.e., m (GO): m (Cu 2 O) of 1:2, 1:5, 1:10, and 1:25, were prepared. When m (GO): m (Cu 2 O) was 1:2, the amount of GO/Cu 2 O nano-composite was 1.00 g/L and C PDS : C DCF was 15:1, and the catalytic degradation rate of diclofenac (DCF) was up to 90%. Corresponding physicochemical properties of the resulting samples were comprehensively characterized by using SEM, TEM, XRD, Raman, FT-IR, and XPS. DCF degradation by activating peroxydisulfate (PDS) via GO/Cu 2 O nano-composite was also investigated in detail. It is found that the synergistic effect, namely GO adsorption and multivalent copper ion electron transfer, makes GO/Cu 2 O nano-composite reveal higher reactivity. Moreover, GO/Cu 2 O nano-composite possesses good stability in consecutive cycling test. EPR analyses shows that ·OH and SO 4 ·− radicals are involved in DCF degradation. It is indicated that the DCF degradation process contain hydroxylation and the cleavage of C-N bond, which is explored by GC–MS. In our research, well-dispersed GO/Cu 2 O nano-composite with high capacity and good cycling stability was fabricated successfully. Compared with pure Cu 2 O nanoparticle, GO/Cu 2 O nano-composite exhibits the better performance for DCF removal. Graphical abstract A novel well-dispersed cuprous oxide (Cu 2 O) deposited on surface of GO was fabricated with high catalytic performance. Its heterogeneous activation of peroxydisulfate (PDS) for diclofenac (DCF) degradation was investigated. GO/Cu 2 O nano-composite was proved high capacity and good cycling stability. Meanwhile, the possible DCF degradation pathway was explored. Compared with pure Cu 2 O nanoparticle, GO/Cu 2 O nano-composite exhibits better performance for DCF removal.
研究领域:
环境科学
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材料科学
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化学工程
·
水处理
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DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2019
·
IF 0
Lijin Huang,Naqing Mao,Qian Yan,Dingwen Zhang,Qin Shuai
Pharmaceutical contamination has drawn tremendous attention because of their adverse effects and potential risks on aquatic organisms and human health. Herein, magnetic covalent organic framework composites (MCOFs) were prepared and utilized for adsorptive removal of diclofenac sodium (DS) from water. The construction of MCOFs was achieved by integrating magnetic nanoparticles (MNPs) into a COFs’ matrix via an organic terracotta process. MCOFs featuring a highly specific area and magnetically separable ability are favorable to DS removal from water. Adsorption equilibrium can be achieved within 20 min following the pseudo-second-order kinetic model (R2 = 0.99). In addition, the experimental data achieved from adsorption isotherms demonstrated that the adsorption of DS onto MCOF-2 can be well fitted by the Freundlich adsorption model, and the maximum adsorption capacity for DS was found to be 565 mg/g. What is more important is that the high removal efficiency of DS from both actual and spiked water samples (>97.0%) was achieved by using MCOF-2 as an adsorbent. Owing to its high stability, the resultant materials exhibited excellent reusability, illustrating the great potential as sorbents for the removal of pharmaceutical contaminants.
研究领域:
环境科学
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材料科学
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药学
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DOI
CHINESE CHEMICAL LETTERS
·
2022
·
IF 8.455
Run Huang,Chaoting Guan,Qin Guo,Zhen Wang,Hanping Pan,Jin Jiang
The large consumption and discharge of diclofenac (DCF) lead to its frequent detection in surface water and groundwater, posing great threats to humans and ecosystems. This study explored the oxidation kinetics of DCF by permanganate (Mn(VII)), and expounded the underlying reason for the unusual pH-dependency that was unclear in previous studies. The kinetics of DCF analogues ( i.e. , aromatic secondary amines) by Mn(VII) oxidation were comparatively investigated. Then, a tentative kinetic model involving the formation of an intermediate between Mn(VII) and DCF or its analogues was proposed to fit the pH-rate profile. Since DCF contained two chloro groups , and a carboxyl group which could be ionized by negative electrospray ionization , a precursor ionization scanning approach was used for the first time for detection of N-containing chlorinated oxidation products. New degradation pathways of DCF containing ring opening, carboxylation , carbonylation , electrophilic addition , hydroxylation and dehydrogenation were proposed based on the identified oxidation products. Moreover, it was demonstrated that the introduction of various reducing agents such as Mn(II), Fe(II) and bisulfite significantly improved the oxidation kinetics of DCF by Mn(VII). The positive effects of Mn(II) and Fe(II) were mainly attributed to the accelerated formation of MnO 2 that acted as a catalyst or co-oxidizer contributing to DCF degradation. The presence of bisulfite caused two-stage kinetics, where a sharp drop of DCF concentration followed by a slowdown of DCF removal. In the first stage, potent reactive manganese species ( e.g. , Mn(III), Mn(V), and Mn(VI)) and sulfate radical were generated during reaction of bisulfite with Mn(VII), whereas bisulfite was depleted fast due to excess Mn(VII) concentrations and the system became the Mn(VII)/MnO 2 system in the second stage. These results provide new insight into reaction mechanism of DCF with Mn(VII) as well as propose a feasible strategy for enhancing the treatment of DCF contaminated water by Mn(VII).
研究领域:
环境科学
·
化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Li Zhang,Yongsheng Fu,Zhenran Wang,Gaofeng Zhou,Runyu Zhou,Yiqing Liu
In this work, the degradation kinetics and mechanism of diclofenac (DCF) using peracetic acid (PAA) activated by zero valent copper (ZVC) were systematically investigated. It was found that PAA could be catalyzed effectively by ZVC to produce HO • , CH 3 COO • and CH 3 COOO • , which were responsible for the removal of DCF. Based on the XPS, XRD and FESEM characterization results of ZVC before and after reaction, the corrosion of ZVC was occurred to produce Cu + under acidic condition, which was the main activator for PAA, H 2 O 2 and O 2 . The recommended pH for this reaction system was 3.0, and DCF degradation was enhanced gradually with increasing ZVC dose and PAA dose. The existence of Cl - , CO 3 2– , Fe 3+ , Cu 2+ and dissolved organic matter (DOM) promoted DCF degradation in ZVC/PAA system, while SO 4 2- and NO 3 – had almost no influence on DCF removal. Six intermediates were identified in this system, and the probable degradation mechanism of DCF was thus proposed, including seven transformation pathways, i.e., hydroxylation, amidation, dechlorination-cyclizaiton, dechlorination-hydrogenation, dechlorination-hydroxylation, decarboxylation and formylation. This study provides a new method for PAA activation and DCF removal from the polluted water.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Chenglong Yu,Erping Bi
Use of reclaimed water for irrigation is a main way for pharmaceutical compounds such as diclofenac getting into the soil environment. However, the role of minerals, especially iron oxides , in the diclofenac adsorption to soils with low soil organic matter (SOM) is still in the lack of evaluation. In this study, adsorption of diclofenac onto six minerals (five nature minerals-hematite, goethite , magnetite, kaolinite and aluminium oxide and one engineered mineral-activated aluminia) and five reference soils was investigated by column chromatography. Adsorption of diclofenac onto minerals and soils was totally reversible and interactions such as H-bonding were the primary mechanisms. Adsorption affinity of iron oxides was much higher than that of nature silicon and aluminum oxides. Diclofenac tended to be adsorbed by mineral surface -OH groups with high thermodynamic stability, which were dehydroxylated at high temperature. Compared with the SOM-dominated sorption of naphthalene , adsorption of diclofenac onto soils was controlled by bonding with surface -OH groups of iron oxides. Adsorption coefficients of diclofenac onto soils can be well predicted by contents of extracted Fe by diethylenetriamine pentaacetic acid (DTPA) instead of total iron oxides contents, suggesting that the bonding was adsorption site-dependent. These findings highlighted the importance of iron oxides in the adsorption of diclofenac (an anionic pharmaceutical compound) in soils with relatively low SOM (e.g., 1.03-3.45%). It also indicated that contents of effective surface -OH groups and DTPA-Fe were the promising parameters to develop the predictive models for diclofenac adsorption onto minerals and soils, respectively.
研究领域:
环境科学
·
土壤学
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DOI
PubMed
高影响因子
Journal of Composites Science
·
2025
·Vol. 9
·期 12
·663
·
IF 3.7
Xiaoyi Gou,Zia Ahmad,Zaijin You,Zhou Ren
The removal of water pollutants with high selectivity and efficiency is still a huge challenge owing to the complex composition of contaminated water. The preparation, modification of Pickering emulsion microspheres, and their application in the adsorption and removal of non-steroidal anti-inflammatory drugs (diclofenac) in water were studied. Poly(2-(diethylamino)ethyl methacrylate-divinylbenzene), (P(DEAEMA-DVB)) microspheres were prepared by Pickering emulsion polymerization. The P(DEAEMA-DVB) polymer was modified with glycidyl trimethylammonium chloride (GTAC) and phenyl glycidyl ether (PGE) to prepare the adsorbent poly(quaternized and phenyl-functionalized) (P(QP-DVB)) with a substantial quantity of quaternary ammonium functional groups. The non-steroidal anti-inflammatory drugs in aqueous solution was mainly adsorbed by the anion exchange interaction with quaternary ammonium species. The adsorption kinetics coincided with the pseudo-second-order kinetic model, and the adsorption isotherm conformed to the Langmuir isotherm model. The optimized P(QP-DVB) particles exhibited well-defined spherical morphology and a uniform particle size distribution ranging from 15 to 30 µm. Nitrogen adsorption/desorption characterization revealed a high specific surface area of 674 m2g−1and a pore size distribution from 2 to 25 nm. In addition, the aforementioned microsphere underwent chemical regeneration and exhibits good reusability, thereby reducing both the economic costs and environmental impacts.
研究领域:
环境科学
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材料化学
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水处理
·
聚合物化学
·
吸附技术
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DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2020
·Vol. 413
·期 1
·193-203
·
IF 3.637
Yang Liwei,Li Lele,Li Fen,Zheng Hejie,Li Tongtong,Liu Xiaoqiang,Zhu Jichun,Zhou Yanmei,Alwarappan Subbiah
Herein, a photoelectrochemical (PEC) aptasensing platform was designed by integrating surface oxygen vacancy (OV) defects, Ti 3+ self-doping, the heterojunction, and resonance energy transfer (RET) effect into one platform for the detection of diclofenac sodium (DCF). Briefly, OV defects were introduced on TiO 2 nanospheres with simultaneous Ti 3+ self-doping, followed by a well-separated deposition of FeVO 4 nanoparticles on TiO 2 to obtain a Ti 3+ -O-TiO 2 /FeVO 4 heterojunction. The surface modification of OVs, Ti 3+ doping, and deposition of FeVO 4 were confirmed by SEM, XPS, EPR, DRS, and PEC measurements. The surface OVs and doping of Ti 3+ species created a new donor (defect) energy level under the conduction band of TiO 2 , which minimized the bandgap and thereby improved the visible light absorption of TiO 2 . Moreover, the capture of photo-excited electrons by surface OVs could hinder the electron-hole recombination. Due to the intimate surface contact and perfect energy matching between TiO 2 and FeVO 4 , the formation of heterojunction decreased the bandgap and facilitated the electron-hole separation of TiO 2 . All these above events contributed to the enhancement of the PEC signals, which were then quenched by the RET effect between Ti 3+ -O-TiO 2 /FeVO 4 and Au nanoparticle (AuNP)–labeled cDNA that had been attached to its complementary DCF aptamer on Ti 3+ -O-TiO 2 /FeVO 4 |ITO. The addition of target-DCF detached AuNP-labeled cDNA from the electrode to recover the photocurrent, resulting in a “signal-on” PEC aptasensor that exhibited a 0.1–500-nM linear range and a detection limit of 0.069 nM for DCF, attributed to the excellent amplification of the proposed aptasensing platform.
研究领域:
分析化学
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环境科学
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材料科学
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电化学
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）