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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

The role of graft-modified chitosan-based coagulants in pharmaceutically combined polluted water: performance and mechanism

Yimu Qiao,Xue Han,Yijia Ren,Feiyong Chen,Cuizhen Sun,Jin Wang,Zhigang Yang,Linxu Xu,Xue Shen,Rupeng Liu

The extensive use of ibuprofen (IBU) and acetaminophen (APAP) has led to their accumulation in surface water, resulting in combined pollution with natural organic matter (NOM). In this study, a novel modified chitosan-based coagulant (CTS-DMDAAC) was successfully synthesized by adding ceric ammonium nitrate (CAN) to make chitosan (CTS) and dimethyldiallylammonium chloride (DMDAAC) produce free radicals for graft copolymerization. The study investigated the effects of pH, initial NOM concentration, and suspended particulates on the performance of contaminant removal and the characteristics of flocs. Through analysis of the Zeta potential and floc characteristics, the primary flocculation mechanisms were identified as: net capture and sweep, charge neutralization, and bridging effect. CTS-DMDAAC demonstrated effective removal of NOM, particularly humus, but encountered challenges in removing small-molecule pharmaceuticals such as IBU and APAP, with removal rates below 15%. To enhance the removal rate of small organic molecules, powdered activated carbon (PAC) was incorporated into the coagulation system, resulting in increased removal rates of IBU and APAP to 71.44% and 79.9%, respectively. Additionally, PAC improved the bridging capacity during coagulation, resulting in a 1.25-fold increase in the strength factor and a 2.34-fold increase in the recovery factor of the flocs. These findings suggest that the combined use of PAC and CTS-DMDAAC presents a novel approach for treating water bodies contaminated with NOM and pharmaceutical complexes.

CAS / MDL: 2158322-33-7
研究领域: 环境科学 · 水处理工程
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Journal of Chemistry · 2024 ·Vol. 2024 ·期 1 ·5515682 · IF 2.8

Efficient Removing of Pharmaceutical Contaminants of Commercial Carbamazepine by Natural Pyrite-Induced Fenton Reaction in a Wide pH Range

Tingting Shi,Jianjun Xi,Yidan Shao,Qiao Tong,Xi Zou,Hongping Zhou,Shourong Liu,Xiaoya Gao

Pharmaceutical contaminants are causing great attention for the public people, urgently requiring to be eliminated from the environment. Herein, commercial pharmaceutical carbamazepine was chosen as a model to be degraded by a heterogeneous Fenton system using natural pyrite as catalyst. The catalyst was characterized by X-ray diffraction apparatus, high-resolution transmission electron microscopy, and X-ray photoelectron spectroscopy. The elements composition and chemical states of pyrite changed significantly after the Fenton reaction, which promoted the production of active species in the electron transfer process. The degradation efficiency of carbamazepine (2.5 mg/L) can reach 99.71% after 30 min with 0.3 g/L of pyrite and 5 mM of H 2 O 2 , respectively. The reaction system was suitable for a wide range of pH (3–9). The environmental adaptability examination of pyrite showed that humic acid (HA) had inhibitory effects on the degradation of carbamazepine. While the changes of degradation efficiency of carbamazepine were inconspicuous in the presence of and , indicating strong anti-interference to environment common anions. Free-radical capturers suggested that hydroxyl radical (∙OH), superoxide radical ( ), and singlet oxygen ( 1 O 2 ) participated in the degradation of carbamazepine. This research has offered a new strategy of “treating wastes with wastes” to use pyrite to remove emerging pollutants.

研究领域: 环境科学 · 药理学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2018 · IF 3.779

Highly efficient and visible-light-driven BiOCl for photocatalytic degradation of carbamazepine

Xiaoya Gao,Wen Peng,Guangbei Tang,Qian Guo,Yongming Luo

Visible-light-driven BiOCl microspheres were directly synthesized via a facile one-pot ethylene glycol mediated solvothermal method. The crystallinity, surface, optical and electronic properties of BiOCl samples were highly depended on the precursor concentration. Benefiting from the exposed (110) facet and oxygen vacancy , BiOCl-10 (synthesized from 0.02 mol of Bi(NO 3 ) 3 ·5H 2 O) displayed a maximum CBZ degradation efficiency of 70% after 180 min under visible light illumination. The reaction kinetics rate constant ( k ) of CBZ degradation in BiOCl-10 (0.0935 min −1 ) was 52 times higher than ordinary BiOCl-1 (0.0018 min −1 ). The improved photocatalytic activities of BiOCl-10 were attributed to the combination of enhanced CBZ adsorption, increased visible light absorption and efficient separation of photogenerated e − - h + pairs. Radicals and holes trapping experiments showed that •O 2 − and h + were predominant active species in the photocatalytic process. Most importantly, BiOCl-10 was also efficient in natural water without any additive. Our findings indicate that the BiOCl-10 photocatalysis can be used as an efficient and cost-effective technology for removal of recalcitrant pharmaceutical contaminants.

CAS / MDL: 501-53-1
研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL TECHNOLOGY · 2023 · IF 2.8

Iron (II) phthalocyanine loaded tourmaline efficiently activates PMS to degrade pharmaceutical contaminants under solar light

Zhendong Wang,Zhexin Zhu,Gangqiang Wang,Xiaoji Ma,Wangyang Lu

Iron (II) phthalocyanine (FePc) is loaded on the surface of the tourmaline (TM) by the reflow method to obtain FePc/TM. This research effectively prevents the π-π stacking of FePc, increased the effective utilization rate of PMS activation under solar light, and further improved the catalytic performance of the catalytic system. The catalytic oxidation efficiency of FePc/TM on carbamazepine (CBZ) and sulfadiazine (SD) can reach 99% under solar light for 15 and 5 min, the total organic carbon (TOC) removal rate can reach 58% and 69% under solar light for 120 min. After 6 cycles, the CBZ removal rate remained above 95%. In addition, the FePc/TM catalytic system has an excellent removal rate for other pharmaceuticals. The results of spin-trapped electron paramagnetic resonance and classical quenching experiments show that FePc/TM can effectively activate PMS to generate active species under solar light, including superoxide radical (•O2−), singlet oxygen (1O2), hydroxyl radicals(•OH), and sulphate radicals (SO4•−). The intermediates of CBZ were identified by Ultra-high performance liquid chromatography and high resolution mass spectrometry, and the degradation pathway was proposed. As the reaction progresses, all CBZ and intermediates are reduced and converted into small acids, or mineralized to H2O, CO2. This work provides an alternative method for the design of efficient activation of PMS activation catalysts under solar light to eliminate residual pharmaceuticals in actual water bodies.

研究领域: 环境科学 · 催化化学 · 污染控制
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CHEMOSPHERE · 2020 · IF 5.778

Self-adjusted bimetallic zeolitic-imidazolate framework-derived hierarchical magnetic carbon composites as efficient adsorbent for optimizing drug contaminant removal

Ying Pan,Qiongjie Ding,Baohong Li,Xiaoxiong Wang,Yiwei Liu,Junhao Chen,Fei Ke,Jianqiang Liu

The construction of efficient and superior adsorbed materials for the precise removal of hazardous contaminants from water have gained significant attention by the scientific community. In this work, a facile bimetallic zeolitic-imidazolate framework (Co x Zn y -JUC-160) by using self-adjusted strategy (SAS) was developed to synthesize various N-doped Co-based hierarchical porous carbon composites through sacrificial template route. A series of highly porous magnetic materials with well-dispersed or reduced Co particle size have been fabricated by fine tuning the ratio of Co and Zn in the precursors. For the first time the effect of the Co/Zn ratio on the textural properties and drug adsorption performance of the resultant porous carbon composites have been investigated systematically. Remarkably, the optimal Co@NC-1/4-900 possesses large specific surface area, hierarchical pore structures, and well-distributed Co adsorption sites which facilitates the exposure of active Co center and realizes fast diffusion of amodiaquine (ADQ) molecules with record-high adsorption capacities (890.23 mg g −1 ). The presented synthetic strategy provides deep insights into the development of highly efficient recyclable magnetic adsorbent for the removal of contaminants.

研究领域: 环境科学 · 材料科学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2018 · IF 4.61

Targeted modulation of g-C3N4 photocatalytic performance for pharmaceutical pollutants in water using ZnFe-LDH derived mixed metal oxides: Structure-activity and mechanism

Guanglan Di,Zhiliang Zhu,Qinghui Huang,Hua Zhang,Jianyao Zhu,Yanling Qiu,Daqiang Yin,Jianfu Zhao

Pharmaceuticals have been frequently detected in various water bodies, posing potential threat to human health and ecological environment. In this work, ZnFe-LDH derived mixed metal oxides (ZnO/ZnFe 2 O 4 , ZnFeMMO) were innovatively adopted to modulate the g-C 3 N 4 photocatalytic performance for the enhanced degradation of ibuprofen (IBF) and sulfadiazine (SDZ) as targeted pollutants. Characterization analyses indicated that the g-C 3 N 4 /ZnFeMMO composites were in the feature of rationally-designed microarchitecture, increased specific surface area, improved light absorbance and efficient charge separation, thereby resulting in promoted photocatalytic activities. Furthermore, the ratio of g-C 3 N 4 to ZnFeMMO in the composites was found to exert significant effects on the resulted microstructures and properties. The results showed that the composite with low g-C 3 N 4 content of 1.0 wt% or high g-C 3 N 4 content of 90 wt% exhibited the optimum catalytic activity for the degradation of IBF or SDZ, respectively. Such distinct structure-activities can be attributed to the different dominated reactive species in two cases: h + for IBF degradation but OH for SDZ degradation. A Z-scheme mechanism was proposed for the charge separation, together with ZnFe 2 O 4 as a light sensitizer. Degradation pathways for IBF and SDZ were established by ESI-QToF-MS technology . This work provided a new perspective to develop rationally-architectured g-C 3 N 4 based photocatalysts for the decontamination of water polluted by pharmaceuticals.

CAS / MDL: 547-32-0
研究领域: 环境科学 · 材料科学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2020 ·Vol. 167 ·期 14 ·143503 · IF 3.721

Electrochemical Degradation of Pharmaceuticals Using Ti/SnO2-Sb2O5-IrO2-RuO2 Anode: Electrode Properties, Performance and Contributions of Diverse Reactive Species

Yijie Liu,Xianzhe Meng,Chao Li,Yifan Gong,Juan Wang,Jiang Bo

Non-biodegradable pharmaceuticals are a group of emerging contaminants that have gained much attention because of their potential risk of inducing adverse ecological and health effects. An efficient Ti/SnO2-Sb2O5-IrO2-RuO2 electrode was prepared by Pechini method and employed as the anode for electrochemical degradation of selected pharmaceuticals (i.e., ibuprofen, atenolol, and carbamazepine). Compared its counterparts, Ti/SnO2-Sb2O5-IrO2-RuO2 exhibited higher oxygen evolution potential, lower chlorine evolution potential, larger active area, and higher stability. Unlike the negligible effect of solution pH from 4.0 to 10.0, increasing current density favored the target pollutants and COD removal. The removal of IBU was mainly attributed to the reaction with •OH, the contribution of which to IBU removal was enhanced with increasing current density. In contrast to IBU, the removal of ATEN and CBZ was mainly ascribed to the reaction with selective radical chlorine species (RCS) mainly in the form of Cl•, which was produced from direct oxidation of Cl− or indirect oxidation by •OH. It was found that the removal of ATEN and CBZ was less affected by dissolved organic matter (DOM) than that of IBU in municipal effluent. This study demonstrates that Ti/SnO2-Sb-RuO2-IrO2 is an attractive electrode for the destruction of pharmaceutical contaminants.

研究领域: 环境科学 · 电化学工程 · 污染控制
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Coatings · 2024 ·Vol. 14 ·期 4 ·439 · IF 2.9

Insights into the Ligand Effect in β-CD@Fe3O4 Composites to Activate Peroxymonosulfate for Efficient Degradation of Pharmaceutical Contaminants: A Study Employing Density Functional Theory

Xi Quan,Pengzhao Lv,Linlin Yin,Wei Zuo,Yu Tian,Jun Zhang

This study presents a detailed investigation into the use of β-cyclodextrin (β-CD) encapsulated iron oxide nanoparticle (β-CD@Fe3O4) composites, modified with different ligands, to activate peroxymonosulfate (PMS) for the degradation of pharmaceutical contaminants, namely, diclofenac, carbamazepine, and erythromycin. The focus is on understanding the ligand effect, particularly using citric acid (CIT), polyethyleneimine (PEI), and cetyl trimethyl ammonium bromide (CTAB), on the degradation performance of these composites. Employing density functional theory (DFT) calculations, this work examines the electronic structure and charge distributions of β-CD@Fe3O4composites, providing insights into their interaction with various pollutants. The study reveals that the β-CD@PEI@Fe3O4composite demonstrates superior degradation efficiency due to optimal electrostatic interactions, regardless of the pollutant’s hydrophobicity. On the other hand, β-CD@CIT@Fe3O4shows moderate efficiency, and β-CD@CTAB@Fe3O4exhibits selective efficiency, particularly for hydrophobic compounds. These findings underscore the significant role of surface chemistry in modulating the activation of PMS and the degradation of contaminants, opening avenues for designing tailored β-CD composites for environmental remediation.

研究领域: 环境科学 · 材料科学 · 理论化学
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International Journal of Environmental Research and Public Health · 2019 ·Vol. 17 ·期 1 ·134 · IF 2.468

Development of Surface Molecularly Imprinted Polymers as Dispersive Solid Phase Extraction Coupled with HPLC Method for the Removal and Detection of Griseofulvin in Surface Water

Kamran Bashir,Zhimin Luo,Guoning Chen,Hua Shu,Xia Cui,Wen Li,Wang Lu,Qiang Fu

Griseofulvin (GSF) is clinically employed to treat fungal infections in humans and animals. GSF was detected in surface waters as a pharmaceutical pollutant. GSF detection as an anthropogenic pollutant is considered as a possible source of drug resistance and risk factor in ecosystem. To address this concern, a new extraction and enrichment method was developed. GSF-surface molecularly imprinted polymers (GSF-SMIPs) were prepared and applied as solid phase extraction (SPE) sorbent. A dispersive solid phase extraction (DSPE) method was designed and combined with HPLC for the analysis of GSF in surface water samples. The performance of GSF-SMIPs was assessed for its potential to remove GSF from water samples. The factors affecting the removal efficiency such as sample pH and ionic strength were investigated and optimized. The DSPE conditions such as the amount of GSF-SMIPs, the extraction time, the type and volume of desorption solvents were also optimized. The established method is linear over the range of 0.1–100 µg/mL. The limits of detection and quantification were 0.01 and 0.03 µg/mL respectively. Good recoveries (91.6–98.8%) were achieved after DSPE. The intra-day and inter-day relative standard deviations were 0.8 and 4.3% respectively. The SMIPs demonstrated good removal efficiency (91.6%) as compared to powder activated carbon (67.7%). Moreover, the SMIPs can be reused 10 times for water samples. This is an additional advantage over single-use activated carbon and other commercial sorbents. This study provides a specific and sensitive method for the selective extraction and detection of GSF in surface water samples.Keywords:dispersive solid phase extraction;griseofulvin;HPLC;removal and analysis;pharmaceutical pollutants;surface water

CAS / MDL: 137234-62-9 22916-47-8
研究领域: 环境科学 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Simultaneous degradation of pharmaceutical contaminants and sterilization in real hospital wastewater by a highly efficient electrocatalytic ozonation process: Performance, mechanism and application

Lingyun Gu,Chunxiu Yu,Kexin Chen,Yi Wu,Xuejie Wang,Heng Zhang,Peng Zhou,Zhaokun Xiong,Bo Lai

Herein, this work investigated an electrocatalytic ozonation (ECO) strategy using stainless steel-graphite plates as cathode–anode for the degradation of the pharmaceutical pollutant dexamethasone (DXMS) and the treatment of real hospital wastewater. The reaction kinetic constant of the ECO degradation of DXMS (0.387 min −1 ) was 4 times higher than that of single ozone (0.087 min −1 ). The established efficient ECO system successfully degraded pharmaceutical contaminants and had excellent bactericidal effects against pathogenic microorganisms ( Escherichia coli ). The results of scavenging experiments, chemical probe experiments, and electron paramagnetic resonance (EPR) analysis indicated that the newly generated 1 O 2 in the ECO system achieved the synergistic effect of the combined EC-ozonation process. More to the point, the ECO system has a high removal rate of chemical oxygen demand (COD) and total organic carbon (TOC) for real hospital wastewater treatment. After 60 min treatment of the ECO system, the COD removal of hospital wastewater ranged from 70 % to 88.91 %, and the TOC removal ranged from 52.05 % to 71.81 %. The ECO system developed in this work has the capacity for simultaneous degradation of pharmaceutical contaminants and sterilization of pathogenic microorganism for hospital wastewater treatment.

研究领域: 环境工程 · 废水处理 · 电化学 · 药学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Laccase-mimicking active inorganic organic hybrid covalent organic framework filtration membrane for rapid removal of drug pollutants

Qixuan Mu,Xinyue Li,Xiuxiu Li,Ruijun Li,Yibing Ji

Designing materials with laccase-mimicking activity are one of the main strategies to overcome harsh operating conditions and expand application modes of natural laccase (Lac). However, achieving their catalytic efficiency ( K cat / K m ) at the level of natural Lac remains challenging. To address these challenges, we designed an inorganic-organic hybrid covalent organic framework (Cu-BSA@COF) with significant laccase-mimicking activity inspired by the concept of “ in situ ” and “restricted coordination”. The combination of organic component (Bovine Serum Albumin, BSA) and inorganic component (Copper) promoted the formation of active centers. XPS confirmed the presence of three valence states of Cu within the material, and BET calculated its specific surface area to be 85.61 m 2 /g. The multivalent copper active centers and high specific surface area provide a basis for laccase-mimicking activity. The synergistic effect of them achieved that the material was essentially identical to natural Lac in terms of substrate affinity ( K m ) and catalytic efficiency. Meanwhile, it also maintained catalytic activity under harsh conditions (temperature, pH, long-term storage, high salt and ethanol concentration). These advantages further promote its integration with membrane technology, thereby achieving the removal of various drug pollutants. The membrane was obtained by the vacuum-assisted process to assemble Cu-BSA@COF onto nylon base film. One constant pressure rapid filtration can remove over 90 % of acetaminophen (APAP), tetracycline (TC), sulfamethoxazole (SMZ), and carbamazepine (CBZ). The wide applicability and effective avoidance of secondary environmental pollution risks provide a new research paradigm for drug pollutants removal.

研究领域: 环境科学 · 材料科学 · 化学工程 · 纳米技术 · 催化
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Electrocatalytic oxidation of ranitidine using a fluorinated blue titanium dioxide nanotube array electrode

Jianhui Xu,Zhijie Cui,Xin Fu,Dan Li,Yanyan Zeng,Yunfei Zhang,Peng Liu,Xiangteng Mo,Kexin Cao,Zijie Shen,Shangkun Ye

Herein, a novel fluorinated blue titanium dioxide nanotube array (F-BTNA) electrode is fabricated via a simple one-step solution immersion method for the efficient electrochemical degradation of ranitidine (RAN), a typical pharmaceutical contaminant in aquatic environment. Characterization reveals that fluorine is successfully incorporated into the TiO 2 lattice, forming stable Ti–F bonds and increasing the contents of surface Ti³ ⁺ (from 53.4 % to 57.8 %) and oxygen vacancies (from 31.04 % to 39.39 %). These modifications enhance the electroactive surface area (from 0.643 to 0.707 m² g −1 ), oxygen evolution potential (from 2.53 to 2.79 V vs. SCE), hydroxyl radical (•OH) yield (from 0.254 to 1.261 mmol min −1 cm −2 ), and interfacial charge-transfer efficiency (from 0.025 to 0.106) compared to pristine TiO 2 (TNA) and blue TiO 2 nanotube arrays (BTNA). The F-BTNA electrode achieves 96.2 % degradation of RAN within 30 min, primarily through •OH-mediated indirect oxidation and direct electron transfer. RAN removal is favored by the presence of Cl – , lower pH and RAN concentration, whereas NO 3 – shows inhibitory effects. Eight degradation intermediates are identified by UPLC-MS/MS, with possible pathways involving C–N/C–S bond cleavage, hydroxylation, and ring-opening reactions. The system achieves 38.3 % TOC removal within 120 min, and toxicity evaluation confirmed that harmful intermediates are further transformed into less toxic products. The F-BTNA electrode exhibits high stability over five consecutive cycles (>86.5 % removal efficiency) and broad-spectrum applicability for degrading various PPCPs. These results demonstrate the F-BTNA electrode's great potential as a practical and robust material for the electrochemical treatment of pharmaceutical-contaminated wastewater.

CAS / MDL: 66357-35-5
研究领域: 环境科学 · 电化学 · 纳米技术 · 水处理技术 · 药物污染 · 高级氧化工艺
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