SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yawen Wang,Jingwen Huang,He Guo,Chendong Puyang,Jiangang Han,Yan Li,Yunxia Ruan
The present study focused on pulse dielectric barrier discharge (DBD) plasma activated persulfate (PS) for sulfamethoxazole (SMZ) degradation in water. The results showed that PS addition could enhance removal efficiency of SMZ in pulse DBD plasma system. The highest removal efficiency, kinetic constant and energy efficiency reached 93.4%, 0.084 min −1 and 0.353 g/kWh respectively with the PS dosage of 40:1 and input power of 85 W. With increase of imput power and pulse frequency, the removal efficiency of SMZ was also increased. The removal efficiency was firstly enhanced and then declined as raising duty cycle and liquid flow rate. SMZ degradation was promoted in alkaline solution conditions. Active species including ·OH, e - , ·O 2 – , 1 O 2 and ·SO- 4 play a certain role in the degradation of SMZ. The decline of O 3 and enhancement of ·OH and H 2 O 2 were found after PS addition. In process of SMZ degradation, the overall conductivity increased but pH decreased. PS addition accelerated the removal of COD and TOC. The degradation process was explored by UV–Vis spectra, three-dimensional fluorescence and LC-MS. Three degradation pathways were deduced based on the indentified intermediates. SMZ degradation in the system was considered as a toxicity-attenuation process. The water matrix including Cl - , HCO 3 – , SO 4 2- and HA have some impact on SMZ degradation. This study presented that pulse DBD plasma could activate PS efficiently, which finally improved pollutant removal efficiency and energy utilization.
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高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Ruotong Jin,Cailian Zhao,Yanxing Song,Xiaojie Qiu,Chenxi Li,Yingxin Zhao
Competitive adsorption and complementary adsorption between emerging pollutants has been observed in multiple studies. Investigation of the preference of pollutants for different types of adsorption sites can provide a supplementary perspective for understanding complementary adsorption. In this study, the simultaneous adsorption of two typical emerging pollutants, sulfamethoxazole (SMX) and bisphenol A (BPA), on magnetic biochar (MBC-1) was investigated. The results showed that the modification with ferric chloride optimized the surface properties of biochar (aromaticity, hydrophobicity , and oxygen-containing functional groups, etc.), and helped to remove SMX and BPA through various interactions. The equilibrium adsorption capacity of the two adsorbents was inhibited by competitive adsorption in the mixed solute systems, which was due to the same adsorption mechanism. When pH = 7, the SMX and BPA adsorption mainly involved pore filling, hydrophobic effect, π-π EDA, and hydrogen bonding. In addition, electrostatic force, surface coordination, and ion exchange have also been proven to be related to the adsorption of SMX and BPA. In the co-adsorption system, BPA's competitive advantage might be due to its superior hydrophobicity, charge property, and molecular diameter. In the competitive adsorption experiment, the total adsorption capacity (Q i ) of the competitive solute exceeded the adsorption inhibition (△Q i ) of the main solute, indicating that the two solutes occupied their preferred adsorption sites, which confirmed the complementary adsorption phenomenon. Complementary adsorption can be explained by the preference of SMX and BPA for different types of adsorption sites. BPA preferentially occupied high-energy sites in the co-adsorption system, such as π-π EDA interaction, ion exchange, and surface coordination. At the same time, SMX tended to be removed by hydrophobic interaction and hydrogen bonding.
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Journal of Water Process Engineering
·
2021
·
IF 5.485
Wen Huang,Yaxin Tang,Xueping Zhang,Ze Luo,Jianqiang Zhang
The pollution problem of livestock manure generated by the rapid development of farming industry is becoming more and more serious, and its conversion into functional materials through a new way is of great practical significance for its resource utilization. For the first time, nano zero-valent iron (nZVI)/biochar composites (Fe-RMC-850) were prepared by carbonizing Fe 3 O 4 -rabbit dung and used to activate PMS for degradation of sulfamethoxazole (SMX). The results showed that Fe-RMC-850 had high catalytic activity due to its rich pore, high graphitization and defective structure. When the dosage of Fe-RMC-850 and PMS were 0.3 g/L and 0.25 g/L respectively, the degradation rate of SMX could reach 100% within 20 min, and it still showed good catalytic stability after 5 cycles of experiments. The radical quenching, EPR and XPS results showed that radical and nonradical pathways acted synergistically in the degradation of SMX, in which nZVI, Fe 2+ -biochar and pyridinic N were used as the main active sites of the radical pathway. The nonradical pathway was attributed to the generation of C-O and COO by the oxygen-containing functional groups on the biochar surface. Moreover, the inherent P atoms formed P C and CPO 3 /C 2 PO 2 , thereby producing defective structures, while the graphitic carbon layer provided good electron transfer sites. Consequently, this study provides a nZVI-rabbit manure biochar composite PMS catalytic material with high organic pollutant degradation efficiency and offers a new option for the resource utilization of manure sources.
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BIORESOURCE TECHNOLOGY
·
2021
·
IF 9.642
Yibo Zhang,Jing Wan,Zhang Li,Zhenbing Wu,Chenyuan Dang,Jie Fu
This study utilized sulfamethoxazole (SMX) acclimatization to enhance the tolerance and biodegradation capacity of Chlorella vulgaris . Compared to wild C. vulgaris , the growth inhibition and oxidative damage induced by SMX evidently decreased in acclimated C. vulgaris , and meanwhile photosynthetic and antioxidant activities were significantly promoted. The physiological analyses with the aid of principal component analysis revealed the increase of catalase and glutathione reductase activities was the critical tolerant mechanism of acclimated C. vulgaris . As the consequence, the acclimated C. vulgaris exhibited enhanced efficiency and (pseudo-first-order) kinetic rate for removal of SMX. The distribution analysis of residual SMX demonstrated the biodegradation was the major removal mechanism of SMX by C. vulgaris , while bioadsorption and bioaccumulation made pimping contributions. During the degradation process of SMX, nine transformation products (TPs) were identified. Based on the identified TPs, a possible transformation pathway was proposed.
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Engineering
·
2023
·
IF 12.8
Ning Li,Haoxi Dai,Mengting He,Jun Wang,Zhanjun Cheng,Beibei Yan,Wenchao Peng,Guanyi Chen
The distribution pattern of metals as active centers on a substrate can influence the peroxymonosulfate (PMS) activation and contaminants degradation. Herein, atomic layer deposition is applied to prepare Cu single atom (SA-Cu), cluster (C-Cu), and film (F-Cu) decorated MXene catalysts by regulating the number of deposition cycles. In comparison with SA-Cu-MXene (adsorption energy ( E ads ) = −4.236 eV) and F-Cu-MXene ( E ads = −3.548 eV), PMS is shown to adsorb preferably on the C-Cu-MXene surface for activation ( E ads = −5.435 eV), realizing higher utilization efficiency. More SO 4 − · are generated in C-Cu-MXene/PMS system with steady-state concentration and 1–3 orders of magnitude higher than those in the SA-Cu-MXene and F-Cu-MXene activated PMS systems. Particularly, the contribution of SO 4 − · oxidation to sulfamethoxazole (SMX) degradation followed the order, C-Cu-MXene (97.3%) > SA-Cu-MXene (90.4%) > F-Cu-MXene (71.9%), realizing the larger SMX degradation rate in the C-Cu-MXene/PMS system with the degradation rate constants ( k ) at 0.0485 min −1 . Additionally, SMX degradation routes in C-Cu-MXene/PMS system are found with fewer toxic intermediates. Through this work, we highlighted the importance of guided design of heterogeneous catalysts in the PMS system. Appropriate metal distribution patterns need to be selected according to the actual water treatment demand. Metal sites could be then fully utilized to produce specific active species to improve the utilization efficiency of the oxidants.
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Journal of the Taiwan Institute of Chemical Engineers
·
2023
·
IF 5.7
Juncao Hou,Jihong Xu,Rui Tang,Yulin Min,Sukum Eitssayeam,Penghui Shi
Background Peracetic acid (PAA) based advanced oxidation processes are of increasing interest due to the generation of organic radical (R-O·) with strong oxidation ability. However, the mechanism of PAA activation by carbon materials is still worth further study. Methods In this study, a series of chicken manure biochar (CBC) materials were prepared at different carbonization temperatures. The active sites and reaction mechanism of biochar materials were studied by the selective quenching method of functional groups. Significant findings High carbonization temperatures endowed CBC with abundant microporous structure. In the SMX degradation experiment, the CBC material prepared at 900 °C (CBC900) allowed complete SMX degradation within 30 min. The degradation rate constant of SMX in the CBC900-activated PAA system was >13 times as high as that in the system activated by benchmark multi-walled carbon nanotubes. R-O· was identified as the dominant reactive specials in CBC900/PAA system and was produced via electron transfer between PAA and CBC900. The defect and oxygen-containing group -COOH was demonstrated as the key active sites to activate PAA. This study provides in-depth understanding of PAA activation by carbon materials and therefore makes contributions to the development and application of PAA-based AOPs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Shenglan Liu,Yongsheng Fu,Guangsheng Wang,Yiqing Liu
In this study, the degradation efficiency and mechanism of sulfamethoxazole (SMX) by UV/sulfite system in presence of oxygen were investigated systematically. The results indicated that SMX could be effectively removed by UV/sulfite following a pseudo first-order kinetic model. Compared to SMX photolysis under UV irradiation, its removal in UV/sulfite system was significantly enhanced, which was mainly ascribed to the formed reactive oxygen species. Sulfate radical (SO 4 − ) was proved to be the major active radical for SMX degradation by scavenging experiments using methanol and tert -butanol as scavengers. UV photolysis and radical oxidation were two degradation pathways of SMX in UV/sulfite system, and their contribution to SMX removal at pH 6.9 was 38.8% and 61.2%, respectively. The degradation rate constant of SMX was decreased from 0.1415 to 0.0358 min −1 as the pH increased from 4.0 to 9.3, because pH is an important influence factor on species distribution of both SMX and S(Ⅳ), further influencing direct SMX photolysis and formation of active species. SMX degradation was increased with the increase of S(IV) concentration from 0 to 1000 μM, while it was decreased with the increase of initial SMX concentration. The presence of HCO 3 − , Ca 2+ and fulvic acid inhibited the degradation of SMX in UV/sulfite system, while an insignificant effect on SMX removal was observed with the addition of Cl − , SO 4 2− and Cu 2+ . NO 3 − could facilitate SMX degradation in UV/sulfite process as a precursor to form hydroxyl radical. Under the direct UV photolysis and radical oxidation, five degradation products of SMX were produced by hydroxylation, S–N bond cleavage of sulfonamide, and oxidation of amino group. Consequently, UV/sulfite could be an efficient approach for SMX removal from polluted water.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2021
·
IF 6.789
Yarui Wu,Hu Cheng,Deng Pan,Liumeng Zhang,Wei Li,Yang Song,Yongrong Bian,Xin Jiang,Jiangang Han
Biochar has been deemed one of the most promising sorbents for the removal of organic pollutants from aqueous solution. In this study, potassium hydroxide-modified Enteromorpha prolifera biochars (PEBCs) were prepared for the first time and applied for efficient sorption of a typical antibiotic, sulfamethoxazole (SMX). The characteristics of PEBCs, including morphology, pore structure, graphitization degree , surface functional groups, and surface element composition, were investigated. Moreover, sorption kinetic and isotherm experiments were carried out to explore the sorption process, performance, and mechanisms. The maximum sorption capacity for SMX can reach 744 mg g −1 , which is much higher than that reported for sorbents. The sorption of SMX onto PEBCs was controlled by both physical and chemical processes. Moreover, pore filling, hydrogen bonding, partitioning, π-π stacking, and electrostatic interactions were possible sorption mechanisms. This study indicated that the structure and properties of algal biochar can be further improved by potassium hydroxide modification at high temperature and applied as an excellent sorbent for the removal of antibiotics from aqueous solution.
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高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2020
·
IF 2.213
Yang Yu,Fei Huang,Yide He,Fuqing Wang,Yong Lv,Yanhua Xu,Yongjun Zhang
Sulfamethoxazole (SMX) is a commonly used antibiotic for both human and animals. The frequent detection of SMX in natural water bodies and sediment has become an issue of great environmental concern due to its potential risk to induce antibiotic resistance in pathogenic bacteria. In the present work, the catalytic wet peroxide oxidation (CWPO) was investigated to remove SMX with sludge-derived carbon (SC) as a cheap alternative catalyst. Different acids were used to modify SC. It was found that SC modified with sulphuric acid (SC-H2SO4) demonstrated the best catalytic activity. The removal efficiency of SMX and TOC was 97.7% and 65.7%, respectively, after 260 min, at pH 5 with a dosage of 220 mg/L H2O2. The effects of temperature, initial pH and H2O2 dosage were also investigated. The study demonstrated that the increase of temperature could significantly improve the degradation of SMX from 10.0% at 20°C to 94.7% at 60°C.
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ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Sijia Kong,Yang-Guo Zhao,Liang Guo,Mengchun Gao,Chunji Jin,Zonglian She
Environmental threat induced by residual antibiotics in marine aquaculture wastewater is an urgent problem to be solved. In this study, one sulfamethoxazole (SMX)-degrading bacterium, Planococcus kocurii O516 was isolated from high SMX marine aquafarm. The isolate was able to consume more than 60% of SMX with the initial concentration of 10 mg L −1 within 72 h. Transcriptome analysis found great gene expression differences in the strains with or without SMX dosage. Three putatively differentially expressed proteins, namely AbrB/MazE/SpoVT family DNA-binding domain-containing protein, pantoate-beta-alanine ligase and MerR family transcriptional regulator, were annotated in detail. They were inferred to trigger the strain’s response to SMX stress. Reverse transcription-quantitative PCR (RT-qPCR) analysis of four significantly different expressed genes accorded well with expression changes revealed by transcriptomics and confirmed the validity of transcriptome analysis. According to functional annotations of the proteins obtained by transcriptome sequencing and structural analysis of the intermediate metabolites by GC-MS, a possible SMX degradation pathway was reasonably proposed. SMX was first decomposed into sulfonamide and 5-methylisoxazole. The sulfonamide was then hydroxylated to form 4-(hydroxyamino) benzenesulfonamide. Subsequently, the sulfamic acid was detached, and 4-(hydroxyamino) phenol was formed. Finally, 4-aminophenol was generated from dehydroxylated of 4-(hydroxyamino) phenol. In sum, transcriptome analysis of the P. kocurii in response to SMX stress benefits to revealing the degradation pathway of SMX and will provide theoretical feasibility for the application of microbial method to treat the SMX-contaminated aquaculture wastewater.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2020
·
IF 3.085
Yan Huang,Li-chao Nengzi,Xiaoling Li,Lezu Meng,Qingqing Song,Xiuwen Cheng
In the study, cuprous oxide (Cu 2 O) combined with sillenite bismuth ferrite (Bi 25 FeO 40 ) was successfully fabricated through hydrothermal strategy. Subsequently, physicochemical properties of Cu 2 O/Bi 25 FeO 40 were studied by X-ray diffraction (XRD), transmission electron microscopy (TEM), N 2 adsorption/desorption, X-ray photoelectron spectroscopy measurements (XPS), UV visible diffuse reflectance spectroscopy (DRS). The experimental results indicated that Cu 2 O/Bi 25 FeO 40 exhibited a significantly enhanced photocatalytic activity , which 85.0% of sulfamethoxazole was decomposed in 120 min under irradiation. Afterwards, scavenger experiments have been carried out to determine the contributions of different species and h + and H 2 O 2 were manifested to be staple reactive species during the process of sulfamethoxazole (SMX) degradation. In addition, Cu 2 O/Bi 25 FeO 40 nanocomposite showed good stabilities. And the degradation efficiency of SMX still reached 84.9% after five recycle experiments. Furthermore, some plausible degradation pathways of sulfamethoxazole were detected by a high-performance liquid chromatography-tandem mass spectrometry. Finally, the enhanced visible light photocatalytic mechanism was proposed reasonably. Eventually, this study provides a novel strategy to prepare catalyst which could be potentially applied in emerging pollutants elimination.
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ENVIRONMENTAL ENGINEERING SCIENCE
·
2015
·Vol. 32
·期 8
·703-712
·
IF 0.991
Ni Liang,Di Zhang,Chaoxian Wei,Hao Li,Saikat Ghosh,Yanbei Cao,Binglin Guo
Organo-mineral complexes are important components of soil and can greatly affect the behavior and fate of organic contaminants. Properties of organic components play important roles in organic coating on mineral surfaces. However, the dominant property and mechanism controlling organic contaminant behavior are still unclear. In this study, adsorption of various organic contaminants on humic acid-nano-Fe2O3 complexes with different properties were investigated. Nonpolar, aromatic, and high-molecular-weight fractions of humic acid (HA) were preferentially adsorbed on nano-Fe2O3, forming various HA-nano-Fe2O3 complexes with different properties. According to a correlation analysis between the adsorption of organic contaminants and properties of HA-nano-Fe2O3 complexes, the organic carbon content, aromaticity, and hydrophobicity, were believed to be the dominant properties controlling the organic contaminant adsorption. Organic carbon contents and π-π bonds might contribute to sulfamethoxazole (SMX) adsorption more than to bisphenol A (BPA) and phenanthrene (PHE) adsorption because the amino functional groups and N-heteroaromatic rings of SMX were strong π-acceptors. In comparison, hydrophobic interactions might contribute to BPA and PHE adsorption more than to SMX adsorption due to the higher hydrophobicity of BPA and PHE. The H-bond was not the dominant mechanism responsible for PHE and BPA adsorption, while it could not be ignored for SMX adsorption.
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