Biochar
·
2022
·Vol. 4
·期 1
·1-19
·
IF 11.452
Han Yu,Gan Lu,Gong Han,Han Jiangang,Qiao Weichuan,Xu Lijie
Metal-free photocatalysts have attracted growing concern recently. Herein, the composites combining g-C 3 N 4 with wood pulp cellulose biochar (WPBC/g-C 3 N 4 ) were synthesized to effectively activate peroxymonosulfate (PMS) under visible light for the degradation of diclofenac (DCF). The incorporation of WPBC endowed g-C 3 N 4 with enhanced visible light absorption, improved charge separation capability, reduced electrical conductivity, and increased photocatalytic and PMS activation capability. Based on quenching tests, electron paramagnetic resonance (EPR), electrochemical analysis and solvent exchange experiments, both radical and nonradical mechanisms were proposed. Radical species including ·OH, h + , ·O 2 – were identified to contribute to DCF degradation. The 1 O 2 and electron transfer were the dominant nonradical pathways for DCF degradation. Moreover, the common influencing factors were examined, and DCF concentration was the most influential factor based on principal component analysis. Generally, the composites exhibited good reusability during consecutive runs. Based on HPLC/MS analysis, four intermediates were detected and the possible DCF degradation pathway was proposed. This work provided a potential strategy based on metal-free WPBC/g-C 3 N 4 for the photocatalytic activation of PMS to effectively degrade emerging contaminants in wastewater. Graphical abstract
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FOOD RESEARCH INTERNATIONAL
·
2025
·
IF 8
Yongfei Zhou,Ning Li,Xinhua Zhou,Li Ming,Hongyan Zhang,Xiaobo Zou,Can Zhang
In this study, we proposed a novel dual-mode paper-based sensor that synergistically combines colorimetric and fluorescence detection for the rapid and sensitive quantification of diclofenac sodium (DFS) in fresh milk, beef, and water matrices. By integrating copper sulfide nanoflowers (CuS) with molecularly imprinted polymers (MIPs), the sensor achieves high specificity and catalytic efficiency, while europium nitrate polymer (EuPMs) enhance sensitivity through fluorescence quenching. The smartphone-enabled analytical platform provides rapid on-site quantification with simplified sample pretreatment, achieving detection limit of 0.007 μM and recovery rates of 95.3 %–114.4 % in real matrices. This innovative approach not only addresses the limitations of traditional methods but also provides a portable, cost-effective solution for monitoring drug residues in agri-food supply chain and agri-environment, bridging the gap between conventional laboratory analysis and field deployable testing.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yunyi Li,Pengfei Gan,Ruihan Jiang,Zhiwei Zhao,Jiangyu Ye,Wen Liu,Meiping Tong,Jialiang Liang
Sulfite [S(IV)] is a promising alternative for sulfate radical-based advanced oxidation processes (SR-AOPs). Transition metal and photocatalysis are generally considered to have a synergetic effect for S(IV) activation. However, the study shows that the synergetic effect is target specific. Herein, an ultra-small Fe 2 O 3 clusters deposited graphitic carbon nitride is synthesized and used for S(IV) activation. For carbamazepine (CBZ) degradation, photogenerated holes can transform S(IV) into sulfate radical and photogenerated electrons can accelerate Fe(II)/Fe(III) cycle, which account for the synergetic effect. In contrast, the degradation of diclofenac (DCF) depends on the excitation of DCF rather than photocatalyst. Instead of radical precursor, S(IV) acts as the electron transfer bridge between excited DCF and photocatalyst. Thus, the deposition of Fe 2 O 3 negatively affects DCF degradation. Density Functional Theory calculation shows that the first excited state rather than the ground state of diclofenac is more suitable for reactive site prediction, which confirms the photosensitization-like degradation mechanism. Moreover, the effects of pH and coexisted anions varies for CBZ and DCF. The study shed light on the synergetic effect of transition metal and photocatalysis for S(IV) activation, and also open an avenue for the study of target specific mechanisms for AOPs.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Sijia Li,Jianan Cui,Xia Wu,Xuan Zhang,Qi Hu,Xiaohong Hou
Metal-Organic Frameworks (MOFs) are efficient adsorbent and catalyst, however, the prepare of MOFs can be extremely time consuming. The rapid in situ microwave synthesis process offers the possibility of MOFs to a large-scale application. In this study, Fe 3 O 4 @MIL-100(Fe) was rapidly prepared via microwave in 30 min using Fe 3 O 4 as metal precursor and applied as the adsorbent and photocatalyst to remove diclofenac sodium (DCF) from water. Fe 3 O 4 @MIL-100(Fe) exhibited an excellent adsorption effect to DCF with the maximum adsorption capacities of 400 mg/L. The presence of H 2 O 2 could promote the removal of DCF during photocatalytic process. Approximately 99.4% of the DCF was removed in Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 system via adsorption removal and consequent photocatalytic degradation . The high efficiency was attributed to the large BET surface area (1244.62 m 2 /g) and abundant iron metal sites (Fe(III) and Fe(II)) of Fe 3 O 4 @MIL-100(Fe). The adsorptive, photocatalytic property of Fe 3 O 4 @MIL-100(Fe) and the Fenton-like reaction were the main mechanisms for DCF removal. TOC analyzer was served to assess the mineralization of solutions treated by Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 in 12 h. High elimination of TOC (87.8%) was observed during the DCF mineralization process. In addition, the major products were illuminated using HPLC-Q-TOF-MS and DCF degradation pathways were also proposed.
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 8
·1-8
·
IF 5.705
Deng Ya’nan,Shen Jiwei,Liu Jiawei,Wei Yinmao,Wang Chaozhan
Poly(2-naphthyl acrylate) was first grafted onto silica-coated magnetic nanoparticles by surface-initiated atom transfer radical polymerization to prepare a reversed-phase magnetic adsorbent. The resulting polymer brush displays enhanced extraction efficiency by offering active sites on the surfaces of adsorbent. It was applied to the preconcentration of the non-steroidal antiinflammatory drugs (NSAIDs) indomethacin (InDo) and diclofenac (DIC). These drugs interact with the sorbent through hydrophobic and π-interactions, and via electrostatic attraction. By coupling the magnetic solid-phase extraction with HPLC, a method for analysis of InDo and DIC in the environmental water samples was established. The limits of detection range from 0.62 to 0.64 ng·mL −1 , and the relative standard deviations for intra-and inter-day analyses of spiked water samples are <11.9%, and relative recoveries are between 62.1 and 96.7%.
A reversed-phase magnetic adsorbent was prepared by grafting poly(2-naphthyl acrylate) brush on the surface of silica coated magnetic nanoparticles. Due to the two conjugated aromatic rings of the monomer, the polymer brush can effectively extract non-steroidal anti-inflammatory drugs through strong π- and hydrophobic interactions.
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Water
·
2024
·Vol. 16
·期 14
·1994
·
IF 3
Hongbin Wang,Shijie Kuang,Youlun Su,Xu Ren,Bowen Yang,Yongliang Sun
Diclofenac (DCF) is often detected in diverse aquatic bodies, and ineffective management can lead to detrimental effects on human health and ecosystems. In this study, degradation of DCF by Fe(III) and Mn(II) activating bisulfite (BS) was investigated. In the Fe(III)/Mn(II)/BS system, 93.4% DCF was degraded at 200 μM BS within 120 s, and additional research on 1000 μM BS achieved 88.4% degradation efficacy. Moreover, kinetics fitting of DCF degradation with the different BS concentrations was studied to find the two highest reaction rates (200 and 1000 μM,kobs= 0.0297 and 0.0317 s−1, respectively). Whereafter, SO4•−and Mn(III) were identified as the main active species at these two concentrations, respectively. Density functional theory (DFT) calculations, molecular frontier orbital theory, and surface electrostatic potential (ESP) forecast electrophilic attack sites. DCF degradation pathways by radical and non-radical ways were proposed by attack site prediction and thirteen intermediates identified by UPLC-QTOF-MS. ECOSAR software 2.2 was used for toxicity assessment. This work studied DCF degradation by the Fe(III)/Mn(II)/BS process in the presence of different concentrations of BS, providing a new insight into water purification.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Zhen Dong,Qiburi Bao,Xin Yang,Zhengkui Zeng,Jifu Du,Long Zhao
Diclofenac sodium (DCF) as an important emerging pollutant has raised significant environment concerns, but conventional adsorbents presented dramatic decline in adsorption capacity under high pH and high salt media. In this work, a vermiculite (VMT) nano-sheet supported ionic liquids (ILs) material was synthesized by two-step involving acid activation and radiation induced grafting 1-vinyl-3-hexylimidazolium tetrafluoroborate onto the VMT (V n -IL, n means the molar concentration of HCl). The V n -IL exhibits above 95% adsorption efficiency at alkaline media. The adsorption isotherms are well obeyed the Langmuir model, with maximum adsorption capacity of DCF onto V n -IL (n=1, 2, 4) determined as 234.75, 245.09 and 255.76 mg/g, respectively, indicating that the adsorption was chemical process. The adsorption efficiency of Vn-IL for DCF was almost not changed, even the concentration of NaCl was 10,000-fold higher than that of DCF. The removal efficiency exhibited negligible reduction after five cycles of regeneration, thereby confirming the stability and recyclability of Vn-IL in DCF elimination.
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TALANTA
·
2018
·
IF 4.244
Chao Wang,Tingxiang Jiang,Kang Zhao,Anping Deng,Jianguo Li
Diclofenac (DCF) is among the pharmaceutical compounds of concern based on its nocuousness in environment. In this work, a novel electrochemiluminescent (ECL) immunosensor for detecting DCF was constructed using poly(etherimide)-poly(3,4-ethylene dioxythiophene): poly(styrene sulfonate) functionalized graphene oxide and CdSe@CdS quantum dots (QDs-PEI-GO/PEDOT) as bioreceptor for conjugating DCF antibody to magnify signal. It is worth noting that this is the first time GO/PEDOT has been applied to ECL sensor field. Compared with GO, GO/PEDOT exhibited a higher conductivity and more stable chemical property, indicating that the proposed immunosensor would possess stronger and more stable luminescence performance. In addition, the electrode was modified with gold nanorods (AuNRs) which increase the load capacity of DCF coating antigen through Au-N bond. Competitive immunoassay method was chosen for structuring immunosensor where polyclonal antibody (pAb) against DCF exhibited high-affinity recognition of DCF, which greatly improved the sensitively and selectivity of sensor. Consequently, the proposed immunosensor gratified in DCF detection with low detection limit (LODs) of 0.33 pg mL −1 (S/N = 3), and displayed high stability and sensitivity, which initiated a new route for DCF determining.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Manli Sun,Qiang Sun,Chuanliang Zhao,Yaoyao Huang,Junyi Jiang,Wei Ding,Huaili Zheng
Given the widespread occurrence of low-concentration diclofenac sodium (DCFS) in the aquatic milieu, the development of an efficient and economical purification method is essential. Magnetic polydopamine-chitosan modified adsorbent (MPDA-CS) was successfully prepared by coating polydopamine-chitosan onto Fe 3 O 4 nanoparticles in this study. The favorable adsorption performance towards DCFS was well demonstrated by regulating the solution to various pH values and initial concentrations of DCFS. Furthermore, the convincing fitting of pseudo-second-order model and intraparticle diffusion model suggested that the dominance of chemical processes and intraparticle diffusion. The specific adsorption mechanism was presumed to be the interaction between MPDA-CS and DCFS molecules, including electrostatic attraction, hydrogen bonding and aromatic stacking. Through regulating standing time in acidic solution, the integrated homogeneous and heterogeneous photo-Fenton system was employed to degrade adsorbed DCFS through dissolved and surfaced Fe(II)/Fe(III) of MPDA-CS, which achieved the waste utilization of dissolved iron ions with excellent degradation efficiency of 96.38% in 40 min. The adsorption-degradation efficiency of DCFS decreased slightly by 2.2% during the initial three cycles. This work presents an energy-efficient method for removing low-concentration DCFS by drawing on the strengths of adsorption and degradation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jiaxin Xu,Huiping Zeng,Jiahao Wu,Yong Chen,Dong Li,Jie Zhang
Economical and eco-friendly chlorine-based advanced oxidation processes (AOPs) have been urgently demanded to enhance the green abatement of emerging micropollutants. Herein, sludge-derived biochar (SBC) was innovatively introduced to activate free available chlorine (FAC) to enhance the elimination of diclofenac (DCF) among pH 5.0–11.0. Pyrolysis of municipal sludge endowed biochar with superior structure, various chemical compositions, and electronic properties, among which carbon-centered persistent free radicals (PFRs) were verified as the dominant active sites for enhanced chlorination based on correlation analysis. Electron spin resonance and electrochemical tests firstly verified that PFRs could mediate electron transfer toward FAC and dissolved oxygen to generate multiple reactive species of •OH, ClO • , 1 O 2 , and O 2 •− . Further investigation revealed that enhanced DCF chlorination relied on both radical attack by •OH, ClO • , O 2 •− and direct electron transfer. Meanwhile, the regeneration of PFRs mediated by FAC and electron-rich DCF greatly promoted the reusability of SBC800. SBC800/FAC system was much superior to sole chlorination in terms of toxicity reduction and anti-interference capacity. This study innovatively introduced SBC as a green and sustainable catalyst to enhance chlorination efficiency, and provided new insights into the activation potential and mechanism of PFRs for chlorination.
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Fanjiang Yang,Siwei Kang,Chao Zhang,Jiaqin Deng,Lu Du,Haoxiang Zhong,Meifang Li,Chunfang Tang,Yuan Ouyang,Zhiming Liu,Zhihang Yuan,Shaohan Li
L-cysteine (L-Cys) is an ideal cocatalyst that enhances the redox cycle of transition metals and accelerates chemical processes, widely used for promoting pollutant degradation in homogeneous systems. However, its role in heterogeneous systems, mechanisms and pathways, remains unclear. In this study, iron-based hydrothermal carbonation carbon (HTCC-Fe) was prepared by reconstituting reed cellulose through hydrothermal carbonization, acid etching, and Fe doping methods. L-Cys promoted the conversion of Fe 3+ to Fe 2+ , which in turn strengthened peroxydisulfate (PDS) activation and increased reactive species formation in the HTCC-Fe/PDS system, with •OH serving as the primary contributor to diclofenac (DCF) degradation, followed by 1 O 2 and O 2 •− . This degradation occurred through pathways including hydroxylation, dehydration, dechlorination, and C–N bond cleavage. As a result, the HTCC-Fe/PDS/L-Cys system achieved a 41.5% higher DCF degradation efficiency than the HTCC/PDS system, coupled with broad pH applicability, strong resistance to anions interference, and effective DCF removal (>70%) in real water matrices. By elucidating the previously unclear role of L-Cys in heterogeneous systems, this work revealed its co-catalytic mechanism in promoting electron transfer and regulating radical/non-radical pathways for enhanced pollutant degradation.
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MOLECULES
·
2023
·Vol. 28
·期 17
·6216
·
IF 4.6
Hongrui Yang,Chen Wang,Wenjuan Zhu,Pingning Jin,Fei Li,Jing Fan
A simple and efficient sample pretreatment technology is very important for the accurate determination of trace drug residues in foods to ensure food safety. Herein, we report a new carboxyl group-functionalized ionic liquid hybrid solid- phase adsorbent (PS-IL-COOH) for the highly efficient extraction and quantitative determination of diclofenac sodium (DS) residue in milk samples. It was found that the adsorption efficiency of PS-IL-COOH for the ppb level of DS was greater than 93.0%, the adsorption capacity was 934.1 mg/g, and the enrichment factor was 620.0, which surpass most of the previously reported values for DS adsorbents. The high concentration of salts did not interfere with the adsorption of DS. Importantly, the recovery of DS was above 90% after 16 adsorption–-regeneration cycles. The synergistic effect of the multiple interactions was found to be the main factor for the high efficiency of DS adsorption. The proposed method was applied to the extraction and detection of DS in milk samples, with the relative recovery ranging from 88.2 to 103.0%.Keywords:carboxyl group-functionalized ionic liquid;solid-phase extraction;diclofenac sodium;milk samples
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