ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 23
·22998-23008
·
IF 2.8
Zhao Junfeng,Wang Qun,Fu Yongsheng,Peng Bo,Zhou Gaofeng
In this study, the effect of Fe 3+ , Fe 2+ , and Mn 2+ dose, solution pH, reaction temperature, background water matrix (i.e., inorganic anions, cations, and natural organic matters (NOM)), and the kinetics and mechanism for the reaction system of Fe(VI)/Fe 3+ , Fe(VI)/Fe 2+ , and Fe(VI)/Mn 2+ were investigated systematically. Traces of Fe 3+ , Fe 2+ , and Mn 2+ promoted the DCF removal by Fe(VI) significantly. The pseudo-first-order rate constant ( k obs ) of DCF increased with decreasing pH (9–6) and increasing temperature (10–30 °C) due to the gradually reduced stability and enhanced reactivity of Fe(VI). Cu 2+ and Zn 2+ ions evidently improved the DCF removal, while CO 3 2− restrained it. Besides, SO 4 2− , Cl − , NO 3 − , Mg 2+ , and Ca 2+ almost had no influence on the degradation of DCF by Fe(VI)/Fe 3+ , Fe(VI)/Fe 2+ , and Fe(VI)/Mn 2+ within the tested concentration. The addition of 5 or 20 mg L −1 NOM decreased the removal efficiency of DCF. Moreover, Fe 2 O 3 and Fe(OH) 3 , the by-products of Fe(VI), slightly inhibited the DCF removal, while α-FeOOH, another by-product of Fe(VI), showed no influence at pH 7. In addition, MnO 2 and MnO 4 − , the by-products of Mn 2+ , enhanced the DCF degradation due to catalysis and superposition of oxidation capacity, respectively. This study indicates that Fe 3+ and Fe 2+ promoted the DCF removal mainly via the self-catalysis for Fe(VI), and meanwhile, the catalysis of Mn 2+ and the effect of its by-products (i.e., MnO 2 and MnO 4 − ) contributed synchronously for DCF degradation.
ᅟ
研究领域:
环境科学
·
化学动力学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yixin Huang,Jinbin Lin,Jing Zou,Jiaxin Xu,Mengyun Wang,Huahua Cai,Baoling Yuan,Jun Ma
Horseradish peroxidase (HRP)-catalyzed hydrogen peroxide (H 2 O 2 ) oxidation could degrade a variety of organic pollutants, but the intrinsic drawback of slow degradation rate limited its widespread application. In this study, 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) was introduced into HRP/H 2 O 2 system as an electron shuttle to enhance diclofenac degradation under neutral pH conditions. The green-colored ABTS radical (ABTS •+ ), generated by the oxidation of ABTS with HRP-catalyzed H 2 O 2 oxidation, was proved to be the main reactive species for the rapid degradation of diclofenac in HRP/H 2 O 2 /ABTS system. There was no destruction of ABTS/ABTS •+ in HRP/H 2 O 2 /ABTS system, and ABTS was verified as an ideal electron shuttle. The reaction conditions including solution pH (4.5–10.5), HRP concentration (0–8 units mL −1 ) and H 2 O 2 concentration (0–500 μM) would impact the formation of ABTS •+ , and affect the degradation of diclofenac in HRP/H 2 O 2 /ABTS system. Moreover, compared with Fenton and hydroxylamine/Fenton systems, HRP/H 2 O 2 /ABTS system had better diclofenac degradation efficiency, higher H 2 O 2 utilization efficiency and stronger anti-interference capacity in actual waters. Overall, the present study provided a meaningful and promising way to enhance the degradation of organic pollutants in water with HRP-catalyzed H 2 O 2 oxidation.
研究领域:
环境科学
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chenghong Qiang,Nan Li,Shixiang Zuo,Zhimin Guo,Wei Zhan,Zhengping Li,Jiangquan Ma
Seeking active and low-cost cocatalysts is a vital task for solving the sluggish kinetics of photocatalysis process in environmental management. Herein, we report a novel and high-efficiency crystallized RuTe 2 cocatalyst, and loaded it onto black TiO 2 to form photocatalytic heterostructure (denoted as RuTe 2 /B-TiO 2 ) for diclofenac (DCF) degradation. To the best of our knowledge, the RuTe 2 as a cocatalyst for photocatalysis based on swift electron capture has not been documented yet. The degradation efficiency of DCF over 0.5% RuTe 2 /B-TiO 2 reached 95.2% for 120 min, which is 1.2 times higher than that of pure B-TiO 2 . In addition, the effects of different calcination temperatures, catalyst amounts, DCF concentrations and solution pH of the as-prepared catalysts were also investigated in depth. Spectroscopy/electrochemistry showed that 0.5% RuTe 2 /B-TiO 2 exhibited a narrower band gap, more active sites and better electrical conductivity than pure B-TiO 2 . Experiments with trapping agents have shown that O 2 – was the main active substance under irradiation. Furthermore, intermediates for the photodegradation of DCF were detected by liquid chromatography mass system (LC-MS) and density functional theory (DFT) calculations. Finally, the degradation pathway was rationalized and a possible photocatalytic mechanism for 0.5% RuTe 2 /B-TiO 2 was proposed.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF PHARMACEUTICS
·
2025
·
IF 5.2
Chenyu Wu,Zijian Wang,Xu Han,Xinyi Yu,Changquan Calvin Sun,Zhengzheng Zhou
Diclofenac (DIC) is a nonsteroidal anti-inflammatory drug with poor tabletability and water solubility. In the present study, a new diclofenac-picolinamide cocrystal (DIC-PIC) was prepared to simultaneously improve its tabletability and solubility. The cocrystal was characterized using multiple techniques, such as X-ray diffraction, thermal methods and spectral analyses. The tabletability of DIC-PIC was significantly improved over DIC, which is attributed to the larger bonding area between crystals due to the higher plasticity of DIC-PIC, demonstrated by the lower in-die mean yield pressure, P y,i , of DIC-PIC (59.5 ± 0.6 MPa) than DIC (86.6 ± 1.4 MPa). The higher plasticity of DIC-PIC is consistent with the existence of a slip plane (001) in its crystal structure. The thermodynamic solubility of DIC-PIC is significantly higher than that of DIC (112 times higher in water and 22 times higher in pH = 6.8 buffer solution). Hence, the simultaneous improvement in tabletability and solubility of DIC-PIC overcomes two main barriers in developing DIC tablets, which makes it a promising candidate for developing a DIC tablet with improved performance.
研究领域:
药剂学
·
药物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Polymers
·
2020
·Vol. 12
·期 1
·72
·
IF 3.426
Qiang Sun,Huaili Zheng,Xuebin Hu,Jun Li,Rui Zhao,Chun Zhao,Wei Ding
In this study, a novel system was set up by preparing a magnetic flocculant combining with ultraviolet/H2O2to realize the rapid enrichment and degradation of diclofenac sodium (DCFS). For the magnetic flocculant, template anion polyacrylamide (TAPAM) with anion micro-block structure was prepared. Thereafter, polydopamine was used to modify TAPAM, Fe3O4nanoparticles was grafted to the modified TAPAM by chelation, named template anion polyacrylamide-polydopamine-Fe3O4(TAPAM-PDA-Fe3O4). Furthermore, the TAPAM-PDA-Fe3O4preparation protocol was optimized by the response surface method (RSM). In the DCFS enrichment section, the rapid separation of flocs from water was realized by an external magnetic field and it indicated that the π–π stacking effect was dominant in neutral/alkaline condition, whereas charge neutralization was favored in acidic conditions. Meanwhile, a DCFS enrichment kinetic curve was much fitted by the pseudo-second-order kinetic model and DCFS enrichment isothermal curve was close to the Freundlich isothermal model, indicating the dependence of DCFS quantity enriched by TAPAM-PDA-Fe3O4and a multilayer heterogeneous enrichment process. The degradation experiment confirmed that DCFS was effectively degraded by ultraviolet/H2O2/TAPAM-PDA-Fe3O4and the maximum value of DCFS degradation efficiency reached 98.1%. Furthermore, the regeneration experiment showed that the enrichment and degradation efficiency of DCFS could maintain a relatively high level in the initial three recycles.Keywords:diclofenac sodium;π–π stacking;charge neutralization;enrichment;degradation
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
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
·
化学工程
✓ 已验证
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 17
·9907-9916
·
IF 3.119
Li Zhang,Yiqing Liu,Yongsheng Fu
In this work, the degradation kinetics and mechanism of diclofenac (DCF) by UV/peracetic acid (PAA) was investigated. The effects of pH, PAA dose and common water components such as inorganic ions and dissolved organic matter (DOM) on DCF degradation by UV/PAA were also evaluated. It was observed that the addition of PAA promoted the photodegradation of DCF due to the generation of reactive radicals in the photolysis of PAA, which was also confirmed by the radical scavenging experiment. The best degradation efficiency of DCF was obtained at pH 8.5. The removal of DCF was enhanced gradually with increasing PAA dose. Since NO3− is a photosensitive substance which can generate HO˙ under UV irradiation, its existence promoted the degradation of DCF. The presence of CO32− could slightly improve DCF degradation, which might be due to the role of generated carbonate radicals. Cl−, SO42− and Fe3+ had little effect on DCF removal, while Cu2+ could enhance DCF degradation because of its catalytic ability for PAA decomposition. An inhibition effect on DCF removal was observed in the presence of DOM, and it was more obvious in higher concentration of DOM. The elimination of total organic carbon (TOC) was low. According to the twelve reaction products detected in the UV/PAA system, the probable transformation mechanism of DCF was proposed exhibiting eight reaction pathways, i.e., hydroxylation, decarboxylation, formylation, dehydrogenation, dechlorination–hydrogenation, dechlorination–cyclization, dechlorination–hydroxylation and amidation. This study indicates that UV/PAA is a promising method for DCF removal from contaminated water.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
·
IF 3.359
Junfeng Zhao,Yiqing Liu,Qun Wang,Yongsheng Fu,Xiaohui Lu,Xiaofeng Bai
In this study, the effect of phosphate, Fe(III), Fe(II), and reductive substances (i.e., Mn 2+ and SO 3 2− ) on diclofenac (DCF) oxidation and its degradation mechanism by Ferrate (Fe(VI)) were investigated. The removal rate of DCF in reaction solution at pH 9.0 adjusted by NaOH (67.36%) was higher than that by phosphate buffer (14.87%) because of the complexation of phosphate with Fe(III) and/or Fe(II) restraining the self-catalysis of Fe(VI). Fe(III) or Fe(II) could significantly catalyze Fe(VI) to generate more intermediates (i.e., Fe(V) and Fe(IV)), whose oxidation capacity was magnitude stronger than that of Fe(VI), leading to the improvement of DCF degradation, besides, the presence of reductive substances, e.g., Mn 2+ and SO 3 2− , could also increase the self-catalysis of Fe(VI), enhancing the removal of DCF, which will be further verified in follow-up studies. Seven oxidation products (OPs) were detected using a quadrupole-time of flight-mass spectrometer coupled with an ultra performance liquid chromatograph (LC-QTOF/MS). Based on these identified OPs, the potential degradation mechanism of DCF by Fe(VI) was proposed showing six reaction pathways, including hydroxylation, decarboxylation, C N bond cleavage, dehydrogenation, formylation, and dechlorination-hydroxylation. This study suggests that Fe(VI) can effectively oxidize and degrade DCF.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
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.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Jiewen Deng,Jieli Ou,Zhenran Wang,Yongsheng Fu,Yiqing Liu
Since limitedly existing researches suggested Cu(II) had deficiently catalytic ability to PAA, in this work, we tested the oxidation performance of Cu(II)/PAA system on diclofenac (DCF) degradation under neutral conditions. It was found that overwhelming DCF removal could be obtained in Cu(II)/PAA system at pH 7.4 using phosphate buffer solution (PBS) compared to poor loss of DCF without PBS, and the apparent rate constant of DCF removal in PBS/Cu(II)/PAA system was 0.0359 min − 1 , 6.53 times of that in Cu(II)/PAA system. Organic radicals (i.e., CH 3 C(O)O• and CH 3 C(O)OO•) were evidenced as the dominant contributors to DCF destruction in PBS/Cu(II)/PAA system. PBS motivated the reduction of Cu(II) to Cu(I) through chelation effect, and then the activation of PAA by Cu(I) was facilitated. Besides, due to the steric hindrance of Cu(II)-PBS complex (CuHPO 4 ), PAA activation was mediated from non-radical-generating pathway to radical-generating pathway, leading to desirably effective DCF removal by radicals. The transformation of DCF mainly experienced hydroxylation, decarboxylation , formylation and dehydrogenation in PBS/Cu(II)/PAA system. This work proposes the potential of coupling of phosphate and Cu(II) in optimizing PAA activation for organic pollutants elimination .
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2019
·
IF 5.714
Shuting Zhuang,Yong Liu,Jianlong Wang
The development of high-efficiency adsorbents and the exploration of their adsorption mechanisms are major challenges in environmental remediation. Herein, MIL-100 was prepared, characterized, and utilized for the adsorptive removal of diclofenac sodium (DCF) from aqueous solutions. A high monolayer adsorption capacity of 773 mg g −1 was recorded. The adsorption mechanism was proposed based on different contributions of two types of pore structure of MIL-100 to the adsorption of DCF from aqueous solutions according to the experimental results and theoretical calculation. During adsorption process, DCF (5.2 × 7.4 × 10.3 Å) diffused through the free area of hexagonal pores (8.6 × 8.6 Å) into the cages of MIL-100, whilst it was adsorbed by the pentagonal pores (4.8 × 5.8 Å) preferentially. Internal mass transfer resistance, which was identified as one of the dominant rate-limiting steps by the mass transfer resistance kinetic models based on the Sips model, will be derived from the diffusion process, which was affected by the size-sieving effect of the pore structure of MIL-100. The successful diffusion of DCF into the interior of MIL-100 and the stable configuration between MIL-100 and DCF accounted for the high adsorption capacity. The capture of DCF into MIL-100 also resulted in the pore size distribution variation of adsorbent, which provided vital experimental evidence for the proposed mechanism. This study may offer deeper insights into other pollutants removal by metal-organic frameworks type adsorbents.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）