Polymers
·
2022
·Vol. 14
·期 4
·720
·
IF 4.967
Xiaoyan Zhu,Jiaqi Tong,Hangzhen Lan,Daodong Pan
Diclofenac sodium (DS), one of the most used non-steroidal anti-inflammatory drugs worldwide, is often detected in wastewater and natural water. This drug is ecotoxic, even at low concentrations. Therefore, it is essential to fabricate low-cost adsorbents that can easily and effectively remove DS from contaminated water bodies. In this study, a polyethyleneimine (PEI)-modified magnetic cellulose nanocrystal (MCNC) was prepared with a silane coupling agent as a bridge. TEM, FTIR, XRD, and VSM were used to demonstrate the successful preparation of MCNC-PEI. This composite adsorbent exhibited efficient DS removal. Furthermore, the adsorption performance of MCNC-PEI on DS was optimal under mildly acidic conditions (pH = 4.5). Adsorption kinetics showed that the adsorption process involves mainly electrostatic interactions. Moreover, the maximum adsorption capacity reached 299.93 mg/g at 25 °C, and the adsorption capacity only decreased by 9.9% after being reused five times. Considering its low cost, low toxicity, and high DS removal capacity, MCNC-PEI could be a promising adsorbent for treating DS-contaminated water.
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2026
·
IF 3.9
Zhang Zutao,Xiao Peiyuan,Mei Jinping,Zhang Xinyu,Dai Anni,Wang Lei,Yao Qiufang
Chlorinated pharmaceuticals like diclofenac (DCF) pose persistent environmental risks due to their bioaccumulation and toxicity, necessitating advanced remediation strategies. Herein, an integrated electrochemical system was developed, combining a self-nitrogen-doped carbon nitride (CN)-supported PdNi (CN@PdNi) cathode for electrocatalytic hydrodechlorination (ECH) with a CN anode for oxidative mineralization in a single, sequential process. The CN@PdNi cathode achieved 98.6% ECH efficiency, selectively cleaving C–Cl bonds to mitigate toxicity, which is attributed to its structural merits, including a well-dispersed, albeit partially clustered, nanoparticle distribution, metallic Pd/Ni phases, predominant Pd 0 /Ni 0 states, and enhanced porosity. Subsequent CN anodic oxidation enabled 96.8% total organic carbon (TOC) removal, ensuring near-complete mineralization. Mechanistic studies via Electron paramagnetic resonance (EPR), quenching, LSV, and Tafel slopes revealed atomic hydrogen (*H) generated at Pd 0 sites as the primary reactive species, augmented by electron transfer. The system exhibited robust performance across varied conditions and exceptional stability (< 1% efficiency loss over 11 consecutive cycles). Toxicity assessments showed 3–5 Log 10 unit reductions (ECOSAR) and mung bean germination rates improving from 68.7 to 99.8%. This dual-functional detoxification-mineralization strategy overcomes the limitations of single-step processes and offers a scalable, sustainable solution for efficient remediation of halogenated pollutants.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Hao-Ze Li,Cheng Yang,Hai-Long Qian,Xiu-Ping Yan
The excessive use of diclofenac sodium (DCF) has led to environmental and food safety problems. Effective removal of DCF in aqueous environment is of great significance. Ionic covalent organic frameworks (iCOFs) are effective adsorbents for the removal of pollutants due to their unique structure and properties, but conventional synthesis of iCOFs is limited by high temperature and long reaction time. Herein, we report a room-temperature strategy to synthesize iCOFs in 24 h for the first time. The room-temperature synthesized ionic COF (RT-iCOF) shows better crystallinity, lager uptake capacity and faster kinetics than those synthesized at high temperature with long reaction time. The adsorption kinetics, isotherms and thermodynamics, the effects of ionic strength, pH, humic acid, and reusability of RT-iCOF for DCF were studied in detail. The prepared RT-iCOF gave the maximum adsorption capacity of 857.5 mg g −1 , featuring the highest uptake capacity for DCF so far. The adsorption of DCF on the RT-iCOF are driven by ion exchange, π-π interactions, electrostatic and hydrogen bonds interaction. The adsorption efficiency of RT-iCOF for DCF was still above 90% after 5 regeneration cycles. This work also promotes the facile synthesis and application of iCOFs for the removal of pollutants.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jieling Song,Wen Liu,Zhaokun Xiong,Bo Lai,Rongfu Huang
This study utilized tetrapolyphosphate (TPP) as the electrolyte in the electro-Fenton (EF) system to efficiently generate reactive oxygen species (ROS) for effective degradation of diclofenac sodium (DCF) by activating dissolved molecular oxygen without aeration. The results indicated that the EF-TPP process produced a higher concentration of Fe(II) ions but a lower concentration of total iron than those concentrations in the regular EF-Na 2 SO 4 process, resulting in the higher degradation efficiency of the former system without producing iron sludge. It was found both hydroxyl ( OH) and superoxide radicals (O 2 − ) are primary reactive species in the EF-TPP system. The EF-TPP system produced a much higher amount of OH (3.886 μmol/L) than that of the EF-Na 2 SO 4 system (0.042 μmol/L). In addition, results of density functional theory (DFT) calculations and characterization experiments revealed the reaction pathway of dissolved molecular oxygen with Fe-TPP complexes, which are primarily present as [Fe(TPP)(H 2 O) 2 ] − and [Fe(TPP) 2 ] 4− in the EF-TPP system. These results indicated that both speciation of Fe-TPP complexes can effectively activate molecular oxygen to generate ROS. DCF degradation pathways were proposed by identifying the formed byproducts. Overall results indicated the electrolyte TPP in the EF-TPP system induces the slow release of iron ions, the formation of Fe-TPP complex to stabilize the Fe(II) in the neutral pH condition, and the enhanced activation of dissolved molecular oxygen via one-electron transfer pathway.
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Hua Guo,Zhicheng Xu,Dan Wang,Shiyu Chen,Dan Qiao,Dan Wan,Hao Xu,Wei Yan,Xiaoliang Jin
This work investigates the electrochemical oxidation (EO) of diclofenac (DCF) in water with Ti/Ti 4 O 7 , Ti/Ru–Ir, Ti/Sb–SnO 2 and Ti/PbO 2 electrodes. Scanning electron microscope and X-ray diffraction results suggest that Ti/Ti 4 O 7 has porous stacked surface morphology and Ti/Sb–SnO 2 possesses the smallest grain size. Linear sweep voltammetry test results indicate that PbO 2 has the highest oxygen evolution potential, while Ti/Ti 4 O 7 and Ti/Ru–Ir show better oxygen evolution activity. DCF degradation results reveal that PbO 2 possessed the highest DCF removal ( R DCF = 99.2%) and chemical oxygen demand (COD) removal ( R COD = 97.0%), the fastest COD degradation rate ( k = 0.0275 min −1 , R 2 = 0.964), the lowest specific energy consumption ( EC DCF = 1.81 kWh . g DCF −1 , EC TOC = 6.90 kWh . g TOC −1 ). The toxicity variation of DCF during EO process on PbO 2 is rise first and then to fall. Considering the differences of the four electrodes in residual, conversion and mineralization aspects, mineralization selectivity ( MS ) was proposed to estimate the mineralization inclination of electrodes during EO process, and PbO 2 displays the strongest mineralization inclination ( MS = 0.594). In addition, the possible degradation pathway of DCF on PbO 2 electrode indicates a composite behavior of conversion and mineralization. All of them above indicate the promising application potential of PbO 2 in lower concentration pharmaceuticals and personal care products wastewater treatment . Moreover, MS could be employed as a supplementary index to assess the different inclinations of this composite behavior on various electrodes used for electrochemical treatment of organics in later studies.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2021
·
IF 7.514
Lijin Huang,Rujia Shen,Ruiqi Liu,Shengrui Xu,Qin Shuai
A robust magnetic solid-phase extraction (MSPE) method based on magnetic covalent organic framework (MCOF) coupled with high-performance liquid chromatography (HPLC)-ultraviolet (UV)/mass spectrometry (MS) was proposed for the determination of trace diclofenac sodium (DS) in milk. The prepared MCOF exhibited high extraction efficiency, which can be attributed to its high specific surface area as well as strong π-π and hydrophobic interactions between MCOF and DS. In addition, the potential influencing factors, including sample volume, adsorbent dosage, extraction time, and elution parameters, were fully estimated. The experimental results demonstrated that the established method was sensitive for the quantification of DS with high accuracy. Remarkably, the detection limit of DS was found to be 10 ng/kg under the optimal conditions. More impressively, the developed method was successfully applied to monitor trace DS in milk, demonstrating its outstanding durability and practical potential as an appealing method to regular monitor trace pharmaceutical contaminants in real food samples.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2020
·
IF 3.99
Xin Mi,Shuangxi Zhou,Ziming Zhou,Mohammadtaghi Vakili,Yue Qi,Ye Jia,Donghai Zhu,Wei Wang
Covalent organic frameworks (COFs) with great application potential in environmental remediation exist as the form of powder, which are difficult to separate and recycle. Two magnetic COFs with good recyclability were prepared through simple impregnation-precipitation method in this study. The prepared magnetic COFs were used for the adsorptive removal of diclofenac sodium (DCF). The introduction of hydroxyl group on magnetic COF (OH-MCOF) could greatly enhance its adsorption amount for DCF, and OH-MCOF was selected to study the effect of adsorption time, initial concentrations, solution pH and ionic strength on its adsorption for DCF, as well as its regeneration and reuse performance were investigated. In this study, the OH-MCOF had a high adsorption capacity for DCF of 203.4 mg/g based on the Langmuir model fitting, and exhibited quickly adsorption for DCF within 30 min. The adsorption efficiency was better than that of most reported adsorbents. Furthermore, the role of hydroxyl group on magnetic COF was highlighted through density functional theory (DFT) and electrostatic potential (ESP) calculation. After 5 cycles of regeneration, the OH-MCOF still maintained the same adsorption amount for DCF, showing good reusability and stability. This study reveals OH-MCOF with high removal and reusability in the further application of environmental remediation.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2019
·
IF 4.784
Yuqing Lu,Ziyi Wang,Xiao-kun Ouyang,Chao Ji,Yonglun Liu,Fangfang Huang,Li-Ye Yang
Diclofenac sodium (DS) is an emerging contaminant that is toxic and remains at high concentrations in natural aquatic environments. The aim of this study was to fabricate a novel spherical polymeric adsorbent composed of cross-linked chitosan beads grafted by polyethylenimine (PEI) to remove DS from water. The adsorbents were thoroughly characterized using Fourier transform infrared spectroscopy , scanning electron microscopy, elemental analyses, and X-ray photoelectron spectroscopy. A cross-linking step was expected to enhance adsorption. The experimental data obtained from a series of adsorption experiments were fit well by the Langmuir isotherm model and pseudo-second-order model. The epichlorohydrin–PEI adsorbent (EPCS@PEI) showed a maximum adsorption capacity of 253.32 mg/g and removal efficiency of nearly 100% for the DS in the initial 50 mg/L solution. Therefore, EPCS@PEI is proposed as a potential adsorbent for DS removal, where these initial findings are expected to promote further design and fabrication of effective adsorbents for practical applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Meixuan Cai,Ruobai Li,Zhijie Xie,Jiaxing Huang,Yongqin Zeng,Qianxin Zhang,Haijin Liu,Wenying Lv,Guoguang Liu
The development of novel noble metal-free semiconductor catalysts with high photocatalytic efficiency is of great importance toward the degradation of organic compounds. In this work, a core-shell heterojunction MoS 2 /Cd 0.9 Zn 0.1 S photocatalytic material was successfully synthesized via a simple one-step hydrothermal method. The introduction of MoS 2 led to a significant improvement in the photocatalytic degradation of diclofenac (DCF). It was confirmed that 0.1% loading content of MoS 2 achieved an optimal photocatalytic efficiency of 86% in the degradation of DCF under visible light irradiation, which was 1.8 times higher than that of Cd 0.9 Zn 0.1 S. The MoS 2 /Cd 0.9 Zn 0.1 S heterostructured composites possessed improved photocatalytic properties, which implied that the combination of Cd 0.9 Zn 0.1 S and MoS 2 shortened the carrier transport pathway and facilitated the separation efficiency of electrons and holes. Reactive species (RS) scavenging experiments and electron spin resonance (ESR) demonstrated that superoxide radicals (O 2 •− ) and electron holes (h + ) played predominant roles throughout the DCF degradation process. The primary intermediates were explored through HRAM LC/MS/MS, and a transformation pathway was tentatively proposed. This study promoted the application of an economical, highly efficient and visible light driven MoS 2 co-catalyst for the degradation of organic contaminants.
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Zhen Chen,Shaoxiong He,Mingshan Zhu,Chaohai Wei
The search for a suitable heterogeneous catalyst in peroxymonosulfate (PMS) activation holds tremendous promise for the degradation of organic pollutants. Two-dimensional (2D) transition metal dichalcogenides such as WS 2 exhibit broad applications in heterogeneous catalysis, and we first extended its application in PMS activation in this work. It was found that WS 2 could efficiently activate PMS resulting in the degradation of diclofenac (DCF). The results show that the PMS offers direct oxidation, and WS 2 could initiate PMS to produce singlet oxygen ( 1 O 2 ) and superoxide radical (·O 2 − ). This resulted in the improved removal of DCF in the WS 2 /PMS system. Furthermore, the degradation pathway of DCF was proposed according to the detected intermediates/products and density functional theory (DFT) calculation. Degradation intermediates and the evaluation of product toxicity indicated that the developed WS 2 /PMS system was a safe and detoxifying process while also offering efficient DCF removal. This study offers more insight into the development of suitable materials for the activation of PMS and gives clear direction for the degradation of DCF and its toxic intermediates.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Jingxin Liu,Hang Jia,Meng Mei,Teng Wang,Si Chen,Jinping Li
Diclofenac (DCF), a widely used drug, is frequently found in natural waters, and its removal has caused extensive concern. Sulfate radical-based advanced oxidation processes are efficient for the degradation of organic pollutants , but the self-decomposition of persulfates is always sluggish and restricted. Herein, self-N doped biochar derived from food waste digestate (FWDB) was evaluated as the activator of peroxylmonosulfate (PMS) in terms of DCF degradation. The effects of several key operating variables were examined, and the results indicated that ∼93% of DCF with an initial concentration of 20 mg/L was removed at FWDB dosage of 0.3 g/L and PMS concentration of 1.0 mM. Thereafter, the machine learning method was explored to simulate and predict the DCF removal process. The reactive oxygen species participated in the reaction was identified as 1 O 2 , and the reaction sites on FWDB were determined as graphitized carbon, C O structure, doped-N, and defective edges. Moreover, based on the identification of intermediates and products, the possible DCF destruction pathways were proposed as hydroxylation , cleavage of N−C bond, and decarboxylation . This study provided an economical and convenient heterogeneous PMS activator for remediation of organic wastewater and confirmed the feasibility of optimizing the contaminant degradation process via data mining .
✓ 已验证
DOI
高影响因子
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2020
·Vol. 20
·期 3
·1807-1813
·
IF 1.134
Wang Yulin,Qiu Xiuzhen,Li Yangyang,Guo Huishi,Lu Wenguan,Nie Libo
A novel molecularly imprinted polymer material based on the metal-organic framework NH2-MIL-101(Cr) (MOF-MIP) was prepared. The synthesized MOF-MIP was characterized by IR, XRD, SEM and N2 absorption. The characterization results displayed that the MOF-MIP which exhibited
an octahedral shape had good dispersibility, good thermal stability and a high surface area. Subsequently, the adsorption behavior of MOF-MIP to diclofenac sodium (DS) in aqueous solution was examined. A series of adsorption experiments demonstrated that the MOF-MIP had high transfer mass
rates and high sensitivity and selectivity for DS. Then the MOF-MIP was used as the adsorbent of dispersive micro-solid phase extraction (DMSPE) for the detection of DS in urine. Under optimum conditions, the average recovery of DS ranged from 88.3 to 101.6% with RSD of 5.6%. The described
method provides a rapid route for determination of DS in human urine.
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）