Antibiotics-Basel
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2022
·Vol. 11
·期 1
·51
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IF 5.222
Xiaoming Su,Hao Lv,Jianyu Gong,Man Zhou
The oxidative mineralization of sulfanilamide drugs (SAs) using micro-size zero-valent iron (mZVI) cooperated with a citric acid buffer solution was evaluated. In this study SM2, SMX, and SD could be removed at 66%, 89%, and 83%, respectively, in a 0.5% Bi/mZVI+CA+NaCA system within 2 h. Based on our analysis, the produced ·OH could be ascribed from the complexation between citrate iron (Fe(II)[Cit]−) and the generated H2O2resulting from the activation of O2on the mZVI surface in the Bi/mZVI+CA+NaCA system, further inducing the mineralization of antibiotics. The related possible degradation pathways were proposed. Two similar degradation pathways of SM2, SMX, and SD in the mixed liquid, including hydroxylation and SO2extrusion, were solved. Meanwhile, there was an additional proposed degradation pathway for SMX to be degraded more effectively, as reflected in the opening of the N-O bond on the benzene ring. Therefore, this work provides an experimental basis and theoretical support for the efficient treatment of antibiotic wastewater in real industry by using an iron-based method.Keywords:sulfanilamide drugs;Bi/mZVI;antibiotic;oxidative degradation
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2023
·
IF 3.8
Kanayo L. Oguzie,Meng Qiao,Emeka E. Oguzie
Anthracene (ANTH) is a difficult to degrade polycyclic aromatic hydrocarbon that can find its way into water bodies through the food chain. In this study, oxidative degradation of anthracene (ANTH) in aqueous solution was undertaken using cobalt ion activated peroxymonosulphate (PMS) that relies on the action of strongly oxidizing sulphate radical anion (SO 4 − ) and hydroxyl radical ( OH). Following the often-reported tendency of natural organic matter to interfere with water treatment interventions, the effect of humic acid (HA) on the oxidative degradation process and efficiency was assessed as well. Results obtained show clearly that Co-activated PMS was very efficient for the degradation of ANTH in water, with complete degradation achieved within 90 min. Degradation was achieved following a 3-stage profile, involving an initial rapid degradation stage, an intermediate slower step and a final steady state degradation state. HA manifested both beneficial and adverse effects on ANTH degradation, modifying the 3-stage degradation mechanism, delaying the process, but not necessarily the final outcome of complete degradation. The local reactivity of ANTH molecule was modelled via quantum chemical computations, which enabled identification of electron-rich regions on the molecule, where attack by oxidizing species would be initiated. This study has shown that the PMS/Co oxidation process is effective for treating anthracene contaminated water, even in the presence of natural organic matter.
研究领域:
环境科学
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化学
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ENVIRONMENTAL POLLUTION
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2019
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IF 5.714
Afzal Ahmed Dar,Jing Chen,Asam Shad,Xiaoxue Pan,Jiayi Yao,May Bin-Jumah,Ahmed A. Allam,Zongli Huo,Feng Zhu,Zunyao Wang
In this study, the degradation of eight bromophenols (BPs), including monobromophenols (2-BP, 3-BP, and 4-BP), dibromophenols (2,4-DBP, 2,6-DBP, and 3,5-DBP), a tribromophenol (2,4,6-TBP) and a pentabromophenol (PBP), by a Fe(VI) reaction process at a pH of 8.0 was systematically studied. It was concluded that their degradation rates increased with increasing Fe(VI) concentrations in solution. The removal of 2,4,6-TBP, 2-BP, and 2,6-DBP was faster than that of the other five BPs, which could be attributed to the position of the substituting Br atom. Moreover, the direct oxidation and coupling reactions greatly influenced the reactivity of the bromophenols with Fe(VI). The electron paramagnetic resonance (EPR) analysis confirmed the presence of hydroxyl radicals in present system. The oxidation reaction products of PBP and 2-BP were recognized by an electrospray time-of-flight mass spectrometer ; hydroxylation, hydroxyl substitution, the cleavage of the C–C bond, direct oxidation and polymerization via an end linking mechanism were noticeably found in the reaction process, resulting in the formation of polymerization products and causing hydroxylation to occur. Theoretical calculations further determined the possible oxidation sites of 2-BP and PBP. This study may provide comprehensive and important information on the remediation of BPs by Fe(VI).
研究领域:
环境科学
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化学
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PubMed
高影响因子
WATER RESEARCH
·
2021
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IF 11.236
Bo Yang,Chengjin Wang,Xin Cheng,Yongli Zhang,Wei Li,Jingquan Wang,Zixin Tian,Wenhai Chu,Gregory V Korshin,Hongguang Guo
The binding between dissolved organic matter (DOM) and micro-pollutants (MPs) results in significant impacts on their migration, transformation and degradation. However, the role of the DOM/MP binding on their oxidative transformation remains poorly studied. The binding of MPs by DOM, in combination with DOM's roles as a photosensitizer and/or a competitor for free radicals, needs to be considered in the context of understanding the DOM's impacts on the oxidative degradation of MPs. This study aims to explore this aspect of DOM/MP interactions based on the quantitation of humic acid (HA) and tetracycline (TET) complexation and its role in TET removal. This study also compared the degradation of free TET versus that bound in HA-TET complexes in different oxidation processes. Fourier transform infrared (FTIR) data show that the carboxyl and phenolic hydroxyl groups in HA are the main binding sites of TET, while nuclear magnetic resonance (NMR) analysis shows the binding of TET engages its -N(CH 3 ) 2 groups, and two-dimensional correlation spectroscopy (2D-COS) data show that the carboxyl groups in DOM are sensitive than phenolic groups in the binding of TET. The difference between the degradation rates (Δk obs ) of the free and bound TET decreased with the increase of ionic strength using sodium nitrate, but increased with the introduction of Ca 2+ and Mg 2+ due to the formation of TET-Ca 2+ /Mg 2+ complexes. Quenching experiments showed that the free radicals (•OH and •SO 4 − ), PMS oxidant and UV light were the main contributors to the TET degradation in UV/PS, UV/PMS and UV/H 2 O 2 processes, respectively. In-situ fluorescence time scanning and differential absorbance spectra showed that free TET was preferentially oxidized over the bound TET in all the tested treatments except UV/PS. These results provide new insights into the role of DOM/MP complexation in the degradation of MPs in natural and engineered systems.
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环境科学
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化学
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BULLETIN OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY
·
2025
·Vol. 114
·期 3
·1-6
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IF 2.2
Huang Zaoquan,Li Xiaoyuan,Hou Siying,Zhao Yanjie,Lu Haijian,Wang Jun,Deng Yirong
To enhance phenanthrene degradation in soil, the effects of four surfactants on the thermal activation of sodium persulfate (SPS) were investigated. Sodium dodecyl diphenyl ether disulfonate (C 12 -MADS) was found to stabilize SPS by reducing the generation of sulfate radicals from its thermal decomposition. Optimal conditions for the surfactant-assisted persulfate system were determined to be 5 g/L of C 12 -MADS at a temperature of 60°C, achieving an 89.80% removal efficiency of phenanthrene in soil. The presence of OH − increased the system pH and decreased the removal efficiency. These results demonstrate that C 12 -MADS significantly enhanced the oxidation of phenanthrene and improves SPS utilization efficiency, contributing to the development of an effective surfactant-assisted persulfate system for soil decontamination.
研究领域:
环境科学
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化学工程
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高影响因子
POLYMER DEGRADATION AND STABILITY
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2025
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IF 7.4
Ranran Qi,Ziwen Gan,Qi Wang,Xiaojie Zhang,Mingyi Liao
In this study, microwave (MW)-assisted oxidative degradation of poly(vinylidene fluoride-tetrafluoroethylene-hexafluoropropylene) (P(VDF-TFE-HFP)) was applied to synthesize carboxy-terminated liquid fluororubber, referred to as LTCFs-246. The resulting product has a carboxyl content of 3.01%, a number-average molecular weight (Mn) of 2100 g/mol, and a polydispersity index (PDI) of 1.61. The product's structure was characterized and analyzed in detail using techniques such as 19 F NMR, UV–Vis, and FTIR spectroscopy. Results indicate that the selective dehydrofluorination reaction (K HF reaction) primarily occurs on four sequence structures: HFP-VDF-HFP, HFP-VDF-TFE, TFE-VDF-HFP, and TFE-VDF-TFE, with similar degrees of reactivity across these structures. Two types of C=C bonds were formed in the LTCFs-246 backbone, primarily through Hofmann elimination and, to a lesser extent, Zaitsev elimination. The oxidative reaction (K C-C reaction) was temperature-dependent. At lower temperatures, H 2 O 2 decomposed slowly, limiting the K C-C reaction; as the temperature increased, H 2 O 2 rapidly decomposed, actively engaging in the K C-C reaction and extensively consuming C=C bonds. Once H 2 O 2 was fully consumed, the K C-C reaction ceased, while the K HF reaction continued uninterrupted. In conclusion, this study provides strong evidence to advance the understanding of the oxidative degradation mechanism of MW-assisted P(VDF-TFE-HFP).
研究领域:
材料科学
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化学工程
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2024
·Vol. 25
·期 23
·12542
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IF 4.9
Yun Ma,Hui Liu,Liuli Zhu,Yi Xie,Chuanqi Ren,Xiaorong Mo,Xiaoying Liu,Chen Liang,Gang Deng,Shuangquan Yao,Chengrong Qin
The thermal washing of oily sludge using sodium persulfate (SD) assisted by sodium lignosulfonate surfactant has been demonstrated to be an effective method for oily sludge remediation. To further explore the underlying mechanisms of this process, a systematic study was conducted by simulating oily sludge systems consisting of saturated hydrocarbons (SaH), aromatics hydrocarbons (ArH), resins (Res), and asphaltenes (Asp). The effects of reaction conditions, such as pH, sodium lignosulfonate alkyl (LSA) concentration, SD concentration, and washing temperature, were analyzed. Furthermore, the oxidative kinetic mechanism during the reaction process was investigated. The results demonstrated that neither petroleum hydrocarbons nor SD underwent significant chemical transformations when exposed to LSA, while SD exhibited a marked oxidative degradation effect on all four types of hydrocarbons. Oxidation kinetics indicated that sodium hydroxide played a catalytic role, with SD being the main oxidant and particularly efficient in degrading Asp and Res. Meanwhile, LSA contributed to the removal of hydrocarbons by reducing the surface tension of the solution, enhancing solubilization. This study not only elucidates the central role of SD in the thermal washing process but also provides a solid theoretical foundation for the practical application of this technology in oily sludge treatment.
研究领域:
环境科学
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化学工程
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Xuerui Yang,Xue Cao,Li Zhang,Yanlin Wu,Lei Zhou,Guangli Xiu,Corinne Ferronato,Jean-Marc Chovelon
The widespread utilization of pesticides has attracted increasing attention to their environmental impacts and effective removal strategies. In the present study, the degradation of herbicides picloram (PCLO) and aminopyralid (AMP) with similar structures were investigated systematically by thermo activated persulfate. Overweight SO 4 •− was determined to be the predominant oxidizing species by quenching experiment. Obtained by laser-flash photolysis (LFP), reaction rate constants of SO 4 •− towards AMP and PCLO were determined at 1.56 × 10 9 M −1 s −1 and 1.21 × 10 9 M −1 s −1 , respectively. Product analysis revealed that both substances underwent similar oxidation paths, namely, successive oxidation on pyridine ring and formation of coupling-products as well as further hydroxylation and decarboxylation . Amino group on the pyridine ring was identified as the main reactive site, which was further confirmed by DFT calculation. It was susceptible attacked by SO 4 •− to form deamination, nitration , and self-coupling products. These couples could be further oxidatively dehydrated to form azo and a series of azo derivatives . EOCSAR program predicted significant hazards on aquatic species during the formation of these couplings and azo derivatives. Our work emphasized the potential ability and toxicity of contaminates to produce azo substances in the presence of amino groups on the pyridine ring.
研究领域:
环境科学
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化学工程
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yake Xu,Lingyu Zeng,Lanqing Li,Yoon-Seok Chang,Jianyu Gong
In this study, we systematically investigated the oxidative degradation of 4-chlorophenol (4-CP) using nano zero valent iron (nZVI, Fe 0 ) cooperated with citric acid (CA), and the role of CA as well as the mechanism of oxidation were deeply evaluated. 56.2% of 4-CP was removed after 60 min under dark condition without any ventilation of oxygen in the presence of Fe 0 and CA. The addition of CA accelerated the release of ferrous ions and promoted the Fenton reaction to generate much more reactive oxygen species (ROS), which was confirmed by EPR. The MINEQL+ 4.6 soft was utilized to calculated the existent species in Fe 0 -CA system, and Fe(II)[Cit] − was found to be the key species playing an important role on the degradation of 4-CP. Fe(II)[Cit] − adsorbed on iron surface accelerated the transportation of electron from Fe 0 to O 2 to produce more OH. This study puts forward the possible mechanism of generating ROS on Fe 0 enhanced by CA and provides an application for the oxidation of pollutants.
研究领域:
环境科学
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化学
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RENEWABLE ENERGY
·
2020
·
IF 6.274
Wang Wenchao,Zhai Yuling,Li Fashe,Li Ying
In this paper, the accelerated degradation and oxidation of Jatropha biodiesel were carried out at 110 °C through the Rancimat method. The applicability of surface tension and UV absorbance in the fuel oxidation degree detection was studied through Gas Chromatography-Mass Spectrometer(GC-MS) and acid value titration. The analysis of experimental data demonstrated that the acid value, surface tension and density of Jatropha biodiesel increased by 551%, 3.8% and 0.91% following oxidation, respectively, while the UV absorption intensity at 230 nm increased nearly 2 times. Subsequently to oxidation, the correlations among surface tension, UV absorbance and acid value of Jatropha biodiesel were 0.9743 and 0.9702. Based on this fact, four prediction models for the degree prediction of fuel oxidation through surface tension and UV absorbance were proposed, while the cross-validation method was utilized. The test analysis finally determined that the two models were Logarithm model and Power model, while the RMESP and R values were 0.093, 0.9875, 0.0705 and 0.9928. Both the accuracy and correlation were high. The acid value prediction model based on surface tension was 7.8%, while the acid value prediction model based on UV absorbance was 3.8%. Both could accurately determine the oxidation degree of biodiesel.
研究领域:
化学工程
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能源科学
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高影响因子
FUEL
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2022
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IF 8.035
Ji Mi,Pengfei Jiang,Yitong Dai,Yiran Zhang,Chongkun Shao,Hujun Xie,Yongsheng Guo,Wenjun Fang
The advancement of propulsion systems accelerates the exploitation and application of various high-energy–density (HED) fuels, and yet severe oxidative-fouling hinders the adoption of such fuels in thermal-stressed conditions. In this work, we investigated the overall thermal-oxidative degradation and deposition process of a typical HED fuel, exo -tetrahydrodicyclopentadiene ( exo -TCD), known as JP-10 (NHOC = 39.6 MJ/L), with the presence of oxygen. The oxidation mechanism of exo -TCD at relatively low temperatures is illustrated on the basis of experimental and computational results. For the first time, the chirality of oxidation products has been discussed, revealing the potential impact of radical configuration on the oxidation process of exo -TCD. Besides, an in-depth investigation on the deposition formation process was carried out by analyzing the structure and composition of polymeric macromolecules with the assistance of TG-IR-GC/MS technique. The oxidative deposition of exo -TCD is illustrated with a three-step mechanism of “oxidation”, “polymerization”, and “deposition”. The solubility of macromolecular species formed upon oxidation is decisive for the deposition propensity of fuels. This work aims to provide a theoretical and methodological basis for the future study on the oxidative stability of HED fuels.
研究领域:
化学工程
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能源科学
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BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Hailian Gao,Jiebin Wang,Meixuan Liu,Shunxin Wang,Wenbo Li,Qingda An,Kunlan Li,Ligang Wei,Chi Han,Shangru Zhai
The aerobic oxidation of lignin model 2-phenoxyacetophenone (2-PAP) in cooperative ionic liquid mixtures (CoILs) with 1-ethyl-3-methylimidazolium acetate ([C 2 C 1 im]OAc) and 1-benzyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([B Z C 1 im]NTf 2 ) was investigated. Complete degradation of 2-PAP was achieved with [C 2 C 1 im]OAc/[B Z C 1 im]NTf 2 molar ratio ( R IL ) of 1/1 and 1/2 at 100 °C for 2 h. The conversion and product yields from CoILs were higher than those in pure ILs, indicating the cooperative effects of [C 2 C 1 im]OAc/[B Z C 1 im]NTf 2 on cleaving aryl–ether bonds. [C 2 C 1 im]OAc promoted the catalytic cleavage of aryl–ether bonds and solvation, and [B Z C 1 im]NTf 2 induced the formation of alkyl radicals and enhanced the product selectivity. Accordingly, the highest conversion of alkali lignin (79.8%) was obtained with R IL of 5/1 at 100 °C for 2 h, and phenol monomers (306 mg/g) were selectively produced. The CoILs exhibited good catalytic capacities for oxidative depolymerization of lignin, which strongly depends on the changes in intermolecular interactions and structural organization with varying R IL .
研究领域:
化学工程
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生物质能源
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环境科学
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PubMed
高影响因子
危险品化学品经营许可证（带存储）