CHEMOSPHERE
·
2021
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IF 7.086
Binghan Xie,Heng Liang,Hong You,Shihai Deng,Zhongsen Yan,Xiaobin Tang
Though sulfamethoxazole (SMX) degradation at the low or medium concentration (SMX< 30 mg/L) has been reported in the microbial fuel cell (MFC), further exploration is still urgently required to investigate how the high concentration of SMX affect the anode biofilm formation. In this study, the degradation mechanism of SMX and the response of microbial community to SMX at different initial concentrations (0, 0.5, 5 and 50 mg/L) were investigated in MFCs. The highest SMX removal efficiency of 98.4% was obtained in MFC (5 mg/L). SMX at optimal concentration (5 mg/L) could serve as substrate accelerating the extracellular electron transfer . However, high concentration of SMX (50 mg/L) conferred significant inhibition on the electron transfer with SMX removal decline to 84.4%. The 16S rRNA high-throughput sequencing revealed the significant shift of the anode biofilms communities with different initial SMX concentrations were observed in MFCs. Thauera and Geobacter were the predominant genus, with relative abundance of 31.9% in MFC (50 mg/L SMX) and 52.7% in MFC (5 mg/L SMX). Methylophilus exhibited a huge increase with the highest percentage of 16.4% in MFC (50 mg/L). Hence, the functional bacteria of Thauera , Geobacter and Methylophilus endowed significant tolerance to the selection pressure from high concentration of SMX in MFCs. Meanwhile, some bacteria including Ornatilinea , Dechloromonas and Longilinea exhibited a decrease or even disappeared in MFCs. Therefore, initial concentrations of SMX played a fundamental role in modifying the relative abundance of predominant populations. This finding would promote theories support for understanding the evolution of anode biofilm formation related to the different initial concentrations of SMX in MFCs.
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高影响因子
Journal of Oceanology and Limnology
·
2020
·Vol. 39
·期 1
·160-172
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IF 0.617
Zhou Xudong,Jiang Xincheng,Gao Shan,Wan Zhenjia,Gao Pengcheng
The increasing use of pharmaceuticals has become a major environmental issue in China. The presence of antibiotics in water may have deleterious effects on non-target aquatic organisms such as microalgae. In this study, a cyanobacterium and an alga species in surface waters, Microcystis aeruginosa and Chlamydomonas microsphaera , were exposed to 0, 0.1, 0.5, 1.0, 2.0, 5.0, 10.0, and 20.0 mg/L of oxytetracycline dihydrate (OXY) and sulfamethoxazole (SMZ) for 96 h to determine the effects of these antibiotics on the growth and surface morphology. Moreover, the photosynthetic activity and the contents of superoxide dismutase (SOD), malondialdehyde (MDA), and protein were measured to examine the biochemical characteristics of M. aeruginosa and C. microsphaera under OXY and SMZ stress. The effects of both antibiotics on the growth of both species were concentration-dependent and characterized by low-dose stimulation and high-dose inhibition. C. microsphaera was more sensitive to both antibiotics than M. aeruginosa was. The algal cell membranes of both species disintegrated after exposure to a high concentration of OXY. All of the physiological parameters measured in this study were relatively stable at low concentrations of OXY and SMZ. After exposure to high concentrations of OXY and SMZ, photosynthetic activity decreased significantly, whereas lipid peroxidation and the abundance of SOD, MDA, and protein increased significantly. Thus, low-dose antibiotics may increase algal blooms in eutrophic waters.
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Journal of Cleaner Production
·
2020
·
IF 7.246
Runyuan Zhang,Xiaoxian Zheng,Bohan Chen,Jinlin Ma,Xiaojun Niu,Dongqing Zhang,Zhang Lin,Mingli Fu,Shaoqi Zhou
An increasing amount of antibiotics has been released into the aquatic environment and caused a serious threat to public health. In this study, a series of magnetic biochars (MBCs) were prepared via one-step graphitization and magnetization for sulfamethoxazole (SMX) removal. The effects of pyrolysis temperature and impregnated FeCl 3 concentration on SMX adsorption were investigated. Characterization of MBC were carried out through SEM, BET, XRD, FTIR, Raman and XPS analyses. The performance for sulfamethoxazole removal was evaluated with the adsorption kinetics and isotherms studies, and the influence of pH, temperature, ion and NOM on SMX adsorption capacity was also examined in batch studies. The results show that the physicochemical properties of the MBCs were dominated by the pyrolysis temperatures and the iron weight ratio. The iron species in MBCs contributed significantly to the enhancement of SMX adsorptive capacity , including increasing the carbonization degree, promoting the formation of oxygen-rich functional groups and providing more adsorption sites. The prepared MBCs was proved to be highly efficient for SMX removal, and the 300-MBC800 was the optimal sorbent with the maximum adsorption capacity of 187.31 mg g −1 , which was 5.3 times of the pristine biochar. The primary mechanisms for SMX adsorption include electrostatic interaction, π-π electron-donor-acceptor (EDA) interaction, hydrogen bonding, and Lewis acid-base electron interactions , mainly resulting from the graphitized structures and enriched functional groups on MBCs. This study demonstrated promise of MBC as an effective and environmentally friendly sorbent for removing SMX from wastewater with high adsorption capacity and cost effectiveness.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Xiaohui Liu,Yongqiang Wang,Shaoyong Lu,Ying Liu,Bin Zhao,Beidou Xi,Xiaochun Guo,Wei Guo,Jian Zhang
This study aims to investigate the removal efficiency and mechanism of sulfamethoxazole (SMX) and fate of corresponding sul genes in an electrolysis-integrated tidal flow constructed wetland system (EC-TFCWs). Compared with the single-stage TFCWs, excellent SMX removal was obtained in EC-TFCWs (increased by nearly 20%) owing to synergistic effect of electrolysis-integrated microbial degradation and flocculation. However, SMX removal in EC-TFCWs can be affected by electrode materials with iron electrode higher removal (average removal efficiency = 81.86%) than that of graphite electrode (average removal efficiency = 77.83%). In addition, the removal efficiency of SMX increased from 65.52% to 84.23%, from 42.32% to 87.22% and from 66.33% to 91.9% with the increase of current intensity from 0.21 mA cm 2 to 1.50 m A cm 2 , hydraulic retention time (HRT) from 6 h to 48 h and electrolytic time from 2 h to 8 h, respectively. This result indicated that the current intensity, electrolytic time and HRT played an important role in SMX removal. The absolute abundance of sul genes in zeolite and effluent in EC (iron)-TFCWs was lower than that of in TFCWs at long stress of SMX. However, iron sludge can become a reservoir of sul genes. A novel EC (iron)-persulfate-integrated TFCWs was developed to further improve the performance of EC (iron)-TFCWs (increased by nearly 10%), which achieved a better removal effect and lower abundance of sul genes than that of in EC (iron)-TFCWs, and SO 4 − played a key important role.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hailun Zhao,Zixuan Zheng,Shangkun Zhu,Ruixin Guo,Yanhua Liu,Jianqiu Chen,Qiulian Yang
Antibiotics are emerging contaminants that have become a global concern because of their refractory and toxic characteristics. The treatment of antibiotic contaminants using advanced electrochemical oxidation processes is currently gaining interest. In this study, we constructed a natural iron-mediated electrochemical system for the removal of antibiotics using natural tourmaline (TM) as the heterogeneous iron catalyst, platinum (Pt) as the anode, and nickel foam (NiF) as the cathode. Sulfamethoxazole (SMX) was selected as the target antibiotic. The surface properties and components of TM were characterized using energy-dispersive X-ray spectroscopy, N 2 adsorption–desorption isotherms, X-ray diffraction, and X-ray photoelectron spectroscopy. Compared with the Pt-NiF electrochemical system, the Pt-NiF-TM electrochemical system showed a 23 times enhanced reaction rate constant of SMX degradation under the optimal conditions of current density 4.17 mA/cm 2 , 200–400 mesh, TM dosage 3 g/L, and initial pH 3, in which SMX was almost completely degraded (removal rate = 99.92 %) after 60 min. The ·OH and ·O 2 – radicals generated in the Pt-NiF-TM electrochemical system were the active species for SMX degradation. Thirteen SMX degradation intermediates were identified and possible SMX degradation pathways were proposed. Density functional theory calculations demonstrated that C3 and N11 are the sites with higher electrophilic reactivity in SMX. Furthermore, toxicity calculations and analysis of SMX and its degradation products showed that after treatment with the Pt-NiF-TM electrochemical system, the toxicity of SMX to the microalgae Oocystis was reduced. Overall, this study provides a novel and environmentally friendly electrochemical system mediated by TM for the highly efficient degradation of antibiotic contaminants.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haiqing Zhang,Richard Lee Smith,Haixin Guo,Xinhua Qi
Ordered mesoporous carbons (OMCs) functionalized with catalytically-active metals have many potential applications in sulfate radical-based advanced oxidation processes for degrading antibiotics. Cobalt cross-linked ordered mesoporous carbon materials (OMC-Co-Tx) were synthesized through evaporation-induced self-assembly, calcinated at (600 to 800) o C. The OMC-Co-Tx materials were then employed as peroxymonosulfate (PMS) activators for removal of sulfamethoxazole (SMX) from aqueous solutions. OMC-Co-T800 prepared by calcination at 800 °C had a large specific surface area (449 m 2 /g), uniform pore structure (∼4.5 nm) and showed the best performance for activation of PMS. With a dosage of 0.1 g/L OMC-Co-T800 and 0.4 g/L PMS, the functionalized OMC material allowed SMX (10 mg/L) removal of up to 99% in 30 min. The increase of calcination temperature promoted the reduction of cobalt in OMC materials and increased the defects in their structure, resulting in better catalyst behavior. Quenching experiments and electron paramagnetic resonance analyses showed that reactive species of sulfamethoxazole degradation involved in the OMC-T800/PMS system were SO 4 •− , OH, O 2 •− and 1 O 2 . HPLC-MS analyses of degradation intermediates formed in the OMC-Co-T800/PMS system allowed elucidation of four transformation pathways for SMX degradation.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yiqing Liu,Shixiang Wang,Zhenran Wang,Yongsheng Fu,Runyu Zhou
A novel FeCu anchored coal gangue (FeCu-CG) composite was prepared by a two-step (acidation and subsequent chemical reduction) method and applied in catalytic activation of peracetic acid (PAA) for sulfamethoxazole (SMX) removal in water. The BET, XPS, SEM , EDS, and XRD characterization of FeCu-CG indicated that it had a porous structure with the S BET area of 36.38 m² g −1 and nano-FeCu particles were successfully loaded in the CG carrier, which provided electrons and Fe(II) for PAA decomposition through the bimetallic corrosion reaction. The hydroxyl radical (HO • ) was verified to be largely responsible for SMX elimination in FeCu-CG/PAA system. More than 96.4 % of SMX was removed by FeCu-CG/PAA in 40 min at initial pH ranging from 5.0 to 9.0. Increasing FeCu-CG dosage from 0.1 to 1.0 g L −1 could enhance SMX degradation in FeCu-CG/PAA system, but higher dosage inhibited SMX removal owing to the aggregation of FeCu-CG particles. Coexisting dissolved organic matter (DOM), HCO 3 - and Cl - suppressed SMX degradation. The degradation pathways of SMX by FeCu-CG/PAA were proffered including hydroxylation, amino oxidation , bond cleavage and coupling reaction based on five detected degradation products .
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Hongmei Zhang,Yuqing Gui,Yan Cao,Min Wang,Benzhi Liu
Molecularly imprinted electrochemical sensor for the detection of sulfamethoxazole was prepared by electropolymerization with sulfamethoxazole as template molecule and o-phenylenediamine as functional monomer. Electrochemical performance of molecularly imprinted sensor was studied by cyclic voltammetry in 0.1 mol/L KCl solution containing 5 μM K 3 Fe(CN) 6 . On the optimal experimental conditions, square wave voltammetry was used to detect sulfamethoxazole. The square wave voltammetric peak current difference of the sensor has a good linear relationship with the concentration of sulfamethoxazole in the range of 0.2to 1.4 μM, and the detection limit is 0.05 μM. The molecularly imprinted sensor has good selectivity, repeatability and stability.
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CHEMOSPHERE
·
2023
·
IF 8.8
Yinxue Li,Bin Wang,Hongru Shang,Yongna Cao,Chunhui Yang,Weijie Hu,Yujie Feng,Yanling Yu
In this study, the effects of various types of key adsorption sites on biochar were investigated on its adsorption capacity for sulfamethoxazole (SMX). The biochar obtained by carbonization of corncob at 800 °C (named CC800) was applied to the adsorption of SMX in aqueous environment. The adsorption of SMX by CC800 exhibited a “Three-stage downward adsorption ladder” characteristic in the whole pH range, which was attributed to the different mechanisms corresponding to different adsorption sites of CC800. The organic solvent method and heat treatment method restored the adsorption sites of CC800 after saturated adsorption. And the results revealed that the pore structure and aromatic structure under acidic conditions, and surface functional groups and pore structure under alkaline conditions were confirmed to be key SMX adsorption sites. The adsorption energies of each adsorption mechanism were calculated by density functional theory (DFT), and their order was (−)CAHB (–COO – ) > π + −π EDA interaction > (−)CAHB (–O – ) > pore filling mechanism > π−π EDA interaction. Based on the above studies, the adsorption performance of biochar to SMX can be improved by targeted modification of its micropore structure, surface functional groups, and aromatic structures.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Hengxin Liu,Haoxi Dai,Shuang Wu,Ning Li,Beibei Yan,Guanyi Chen
Persulfate (PS) activated by thermal or homogeneous metals can generate reactive oxygen species (ROS) and high-valence-state metals for contaminants degradation, showing great potential for applications. However, thermal effect in peroxymonosulfate (PMS) system with high-valence-state metal is still ambiguous. In this study, divalent copper (Cu(II)) catalysis was taken to explore thermal effect on PMS performance. Results showed that the Sulfamethoxazole (SMX) removal efficiency in the Cu(II)/PMS system at 60 min increased by only 5.9% with temperature increase from 30 °C to 60 °C. Moreover, SMX removal efficiency was excellent at neutral or basic pH, best with PMS concentration of 2.4 mM, and slightly affected by Cu(II) concentration. The singlet oxygen ( 1 O 2 ) was identified as main active species at low temperature while sulfate radicals (SO 4 − ) was more effective at high temperature with Cu(II) co-activation. Also, trivalent copper (Cu(III)) was an important active species. The higher Cu(III) content, the better SMX removal efficiency, but the stronger intermediates toxicity. In combination with removal efficiency and intermediates toxicity at different temperatures, 30 °C was the optimal reaction temperature. Overall, this study provides new perspective on utilization of waste heat and high-valence-state metal for organic wastewater treatment in PMS systems.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2019
·
IF 3.131
Mi Wu,Shifeng Zhao,Mingxiu Tang,Ruisen Jing,Yifei Shao,Xijuan Liu,Yuanpeng Dong,Mingzhu Li,Qiang Liao,Guocheng Lv,Qian Zhang,Zilin Meng,Aiju Liu
The contaminantsin environment generally do not exist alone and possess different physical and chemical properties, their environmental behavior and mechanism of action in environment are more complicated. Montmorillonite was employed as adsorbent to remove tetracycline (TC) and sulfamethoxazole (SMZ) respectively and simultaneously under batch kinetic and different solution conditions. As the contaminant present singly, it only had a good effect to TC removal. The experimental data were well fitted to pseudo-second-order kinetic model, and the adsorption behavior followed the Langmuir isotherm indicated that TC adsorption was a monolayer coverage and charge-limited adsorption process . In addition, the TC molecular arrangement in the interlayer were analyzed experimentally and through simulation. While the contaminants co-exist, not only TC but also SMZ was removed effectively. SMZ adsorption mechanism were investigated through adsorption equilibrium experiment, characterization and molecular dynamics simulation . Experiment data showed that the best agreement was obtained with the Freundlich model and the adsorption mechanism was proved that SMZ was trapped by hydrophobic interaction.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Shizong Wang,Jianlong Wang
The effect of common inorganic anions (chloride, bicarbonate, carbonate, nitrate, sulfate and phosphate) on the radiation-induced degradation of sulfamethoxazole (SMX) was investigated. In the absence of anions, the removal efficiency of SMX reached 99.6% at dose of 1 kGy. However, the presence of inorganic anions had obvious influence on SMX degradation, which was dependent on their initial concentrations. Nitrate ions had inhibitive effect, which increased with increase of its initial concentration. Chloride ions showed no obvious inhibition at low concentration, while they had significant inhibition at higher concentration. For bicarbonate, carbonate and phosphate ions, they presented inhibition at low concentration, while they had enhancing effect at higher concentration. The promotion of SMX removal efficiency was observed when the initial concentration of bicarbonate, carbonate and phosphate was 50, 20 and 50 mM, respectively. Quenching experiments proved that hydroxyl radicals made a major contribution to SMX degradation in the absence of anions. However, in the presence of 50 mM of carbonate or phosphate ions, carbonate and phosphate radicals played a key role in SMX degradation. In addition, carbonate and phosphate radicals preferentially attacked the amino group and resulted in the formation of different intermediate products compared to hydroxyl radicals. The results suggested that the effect of inorganic anions on the radiation-induced degradation of sulfonamides antibiotics should be considered when radiation technology is used for the treatment of industrial wastewater.
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