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SCIENCE OF THE TOTAL ENVIRONMENT · 2023 · IF 9.8

Enhanced chlorination of diclofenac using ABTS as electron shuttle: Performance, mechanism and applicability

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 .

研究领域: 环境科学 · 水处理工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2016 · IF 3.782

Interfacial thermodynamics and kinetics of sorption of diclofenac on prepared high performance flower-like MoS2

Yalei Zhang,Zengfu Yin,Chaomeng Dai,Xuefei Zhou,Wen Chen

Flower-like MoS 2 with numerous wrinkled nanosheets was prepared via a facile hydrothermal method . The surface morphology and microstructure of the obtained materials were characterized using X-ray diffraction data (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). Additionally, the compositions of the flower-like MoS 2 were further revealed by an energy dispersion spectrometer (EDX) and X-ray photoelectron spectrometry (XPS). The obtained MoS 2 was used as an adsorbent to remove diclofenac (DCF, C 14 H 10 Cl 2 NO 2 Na) from aqueous solutions and presented excellent performance for removing DCF. The sorption kinetics, isotherms and effect of solution pH on the sorption were evaluated in batch sorption experiments. The sorption characteristics of the interactions between DCF and MoS 2 in water were analyzed using a pseudo-second-order model, an intraparticle diffusion model and Boyd model to determine the sorption rate-determining steps. It was concluded that the sorption of DCF on MoS 2 was fitted better by the pseudo-second-order model and that external diffusion governed the sorption process of DCF onto the MoS 2 . The interfacial interaction free energies between DCF and MoS 2 in the sorption process can be calculated based on the extended Derjaguin–Landau–Verwey–Overbeek (XDLVO). The flower-like MoS 2 presenting excellent performance for removing DCF, could be a better choice of treating DCF-containing wastewaters.

研究领域: 环境科学 · 材料科学
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CHEMOSPHERE · 2019 · IF 5.108

Degradation of diclofenac by Fe(II)-activated bisulfite: Kinetics, mechanism and transformation products

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.

CAS / MDL: 15307-79-6
研究领域: 环境科学 · 化学
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Journal of Water Process Engineering · 2025 · IF 6.7

Simultaneous removal of diclofenac, triclosan, and microplastics using graphene oxide-chitosan sponges

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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INDUSTRIAL CROPS AND PRODUCTS · 2024 · IF 5.6

Cationized lignocellulose-based composite aerogel features anisotropic and honeycomb-like structures for efficient removal of diclofenac sodium from water

Fajian Zeng,Gege Cheng,Xing Zhou,Liangyi Yao,Qin Huang,Yan Jiang,Xiuyu Liu

Composite aerogels (CPA) constructed based on lignocellulose nanofibers (LCNF) with anisotropic and honeycomb-like three-dimensional network structures are excellent adsorbent materials. LCNF, as a core constituent of CPA, combines the advantages of cellulose nanofibers and lignin, which endows excellent adsorbent properties to the aerogels and shows great potential in the adsorption of aromatic pollutant diclofenac sodium (DS). Herein, a deep eutectic solvent (DES) and high-pressure homogenization strategy was employed to prepare cationized lignocellulose nanofibers (CLCNF) from industrial and agricultural waste bagasse, and cationized lignocellulose-based composite aerogels were prepared with polyvinyl alcohol (PVA) as crosslinking agent combined with directional freezing technique to efficiently remove DS from water bodies. The prepared CPA had a uniformly distributed honeycomb-like pore structure (porosity ≈ 98 %) and excellent mechanical properties (compressive strength up to 183.93 KPa). In addition, the CPA had a rapid adsorption response to DS with a theoretical maximum adsorption capacity of up to 298.51 mg/g. Its adsorption behavior was in accordance with the pseudo-second order kinetic and Langmuir isotherm model, which demonstrated that it was dominated via the monolayer chemical adsorption, and the main mechanism of the adsorption were electrostatic interactions and intermolecular interactions. Importantly, the CPA still had good stability and reusability after four cycles of use. Therefore, the CPA prepared in this study can be used as a desirable adsorbent for water remediation to achieve the effect of "treating pollution with waste".

研究领域: 环境科学 · 材料科学
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