BIORESOURCE TECHNOLOGY
·
2019
·
IF 6.669
Shengnan Li,Tao Hua,Chung-Shin Yuan,Baikun Li,Xuya Zhu,Fengxiang Li
s Sulfamethoxazole (SMX) is a general antibiotic that is frequently identified in wastewater and surface water. In this study, the degradation and metabolic pathway of SMX by bio-electro-Fenton systems equipped with a CNT/r-FeOOH cathode were investigated. When initial SMX = 25 mg/L, the removal efficiency of SMX reached 94.66% by the bio-electro-Fenton system. The concentrations of sul 1, sul 2, sul 3, sul A , intI 1 and 16S rRNA genes were examined in effluents. Four out of the six ARGs analysed were detected. Among all quantified sul genes, sul 1 and sul A were the most abundant. High-throughput sequencing revealed that the microbial communities and relative abundance at the phylum and genus levels were affected by different SMX concentrations. In addition, the intermediates were detected and the possible SMX degradation pathway by the bio-electro-Fenton process in the present system was proposed. Furthermore, the highest power density obtained was 283.32 ± 16.35 mW/m 2 (SMX = 25 mg/L). This study provides an efficient and cost effective method for degrading antibiotics.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Shizong Wang,Lejin Xu,Jianlong Wang
Nitrogen-doped graphene (NRGO) can activate peroxymonosulfate (PMS). However, the activation mechanism of PMS by NRGO needs to be further investigated. In this study NRGO was prepared by a facile method, and its activation mechanism of PMS for the degradation of sulfamethoxazole (SMX) was investigated. The XPS spectrum showed that nitrogen loading reached 16.5% (atomic percentage). The SMX removal efficiency reached 91.7% at 240 min in the NRGO-activated PMS system. During the PMS activation process, NRGO acted as dual roles: PMS activator and electron transfer mediator. NRGO can activate PMS to form singlet oxygen. In addition, NRGO can act as the electron transfer mediator to enhance the SMX degradation. Density functional theory (DFT) calculations demonstrated that nitrogen doping increased the charge density of net positive carbon atoms and decreased the energy gap, further enhancing the PMS activation. The effects of pH, temperature and the concentrations of chloridion and humic acid were investigated. NRGO had good stability in activating PMS evidenced by the cycling experiments. Eight degradation intermediate products of SMX was identified. Among them, 3-amino-5-methyl-isoxazole and 4-nitro-SMX presented high abundance. The acute toxicity of treated SMX solution increased, suggesting that the degradation products of SMX formed in the non-radicals’ process should be concerned. This study provided an insight into the SMX degradation by NRGO-activated PMS including the mechanisms of PMS activation and SMX degradation.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Pingping Yan,Qian Sui,Shuguang Lyu,Hongyuan Hao,Horst Friedrich Schröder,Wilhelm Gebhardt
Fe(II) activated sodium percarbonate (SPC) process (SPC/Fe(II)) could efficiently remove sulfamethoxazole (SMX) in the aqueous phase, and has the potential in groundwater remediation . However, the degradation mechanisms, especially the degradation products and pathways till now have remained unclear. In the present study, intermediate products were identified using high resolution liquid chromatography coupled with ion trap and time-of-flight mass spectrometry (LCMS-IT-TOF). Nine intermediate products were identified, six of which have not yet been reported during the oxidation of SMX. The oxidation mechanisms involved hydroxyl substitution, the cleavage of sulfonamide bond, isoxazole ring opening and a rearrangement following the loss of the SO 2 -group. Based on the identified intermediate products, the degradation pathways of SMX by SPC/Fe(II) process were illustrated. Fenton's reaction after the dissolution of SPC was proposed as the main reaction mechanisms, which was checked and confirmed by radical species detection tests and radical species scavenging studies. The results showed that although both O 2 − and HO were present in SPC/Fe(II) system, HO was dominant in the system while O 2 − was seldom involved in the degradation of SMX. These findings provided useful information and supported the application of this advanced oxidation process for antibiotics elimination in the groundwater.
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RSC Advances
·
2018
·Vol. 8
·期 49
·27623-27630
·
IF 2.936
Xiaoli Huang,Qi Hu,Lei Gao,Qirui Hao,Peng Wang,Dongli Qin
A metal–organic framework, MIL-101(Cr), was used to adsorb sulfamethoxazole (SMZ) in water and activated persulfate (PS) oxidation was investigated to regenerate SMZ-saturated MIL-101(Cr). Adsorption and oxidation were combined in this study. MIL-101(Cr) was characterized by SEM, BET, XPS and FT-IR analyses. Effects of various operating parameters on adsorption efficiency were studied. The dosages of persulfate for SMZ desorption and oxidation were investigated. The results showed that the recommended pH was 6–8 for SMZ adsorption and optimum MIL-101(Cr) dosage was 0.1 g L−1. SMZ adsorption by MIL-101(Cr) was a spontaneous process and nearly exothermic. Saturation adsorption capacity was achieved in 180 s and the adsorption followed the pseudo-second-order model. The maximum adsorption amount of MIL-101(Cr) to SMZ was 181.82 mg g−1 (Langmuir). MIL-101(Cr) also showed good adsorption capacities for sulfachloropyridazine (SCP), sulfamonomethoxine (SMM), and sulfadimethoxine (SDM). Persulfate was helpful for SMZ desorption from the surface of saturated MIL-101(Cr) and sufficient persulfate could simultaneously oxidize the SMZ. XPS analysis showed that the structure of MIL-101(Cr) was stable after the persulfate oxidation process. Regenerated MIL-101(Cr) had the same level of adsorption capacity as fresh MIL-101(Cr). An adsorption–oxidation combined process may be set up based on the results. This study provides basic data for the deep treatment of organic micropollutants in urban water bodies.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Han Zhang,Siyu Deng,Luxiang Zhu,Yanan Liu
The ubiquitous presence of sulfonamides (SAs) in wastewater poses serious risks to human health and ecosystem safety. This study evaluated the performance of a falling film dielectric barrier discharge (DBD) system on the removal of five SAs, namely sulfamethoxazole (SMX), sulfisoxazole (SIZ), sulfathiazole (STZ), sulfadiazine (SDZ) and sulfamerazine (SMR). Removal efficiencies >99 % were observed for all target SAs within 30 min of treatment, with pseudo-first order rate constants varying between 0.17 and 0.27 min −1 . Superior removal efficiencies were achieved under acidic conditions compared to neutral and alkaline conditions. Using SMX as a model compound, mechanistic investigations revealed that the synergy of reactive oxygen species (ROS) and reactive nitrogen species (RNS) led to its efficient degradation, with peroxynitrites (ONOO − /ONOOH) and hydroxyl radical (OH ) playing pivotal roles. SMX degradation pathways encompassing nitration/nitrosation, hydroxylation, deamination, C S and S N bond cleavage were proposed. The toxicity evaluation results demonstrated that the solution toxicity diminished following the plasma treatment under specific conditions. In particular, the solution treated with air or oxygen discharge enhanced the growth of wheat seedlings, suggesting the potential for reusing plasma-treated wastewater in agriculture. This study enhances our understanding of the underlying mechanisms involved in the plasma degradation of SAs and reveals the significant potential of plasma technology as a sustainable approach for treating wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yali Song,Ziyan Li,Cairong Yang,Xiaojing Zhang,Qiong Wang,Xiaoyu Wen,Hongzhong Zhang,Long Huang
A simple method for preparing C self-doped g-C 3 N 4 (CCN) was proposed by calcining urea and barbituric acid to effectively degrade sulfamethoxazole (SMX). X-ray photoelectron spectroscopy and element content analysis implied C atom replaced the original position of the bridging N atom to form CCN. Compared to g-C 3 N 4 , the absorption edge of CCN was red-shifted. As a result, the band gap of CCN was reduced, which improved the light absorption capacity of CCN and the separation efficiency of photogenerated electron-hole. Ultimately, the photocatalytic activity of CCN was finally boosted. CCN can effectively degrade SMX under visible light. Among CCN with various C dosage, when 0.05 g of barbituric acid was added in the preparation process, the obtained sample (CCN-0.05) exhibited uppermost degradation efficiency on SMX, which can reach 99.0 % after irradiation for 60 min. Additionally, the first-order kinetic reaction rate constant (0.086 min −1 ) was 8.9 times higher than that of g-C 3 N 4 (0.0097 min −1 ). Electron paramagnetic resonance and trapping experiments showed that the dominant reactive species on SMX degradation were surface ·O 2 − and photogenerated holes by CCN-0.05 under visible light. Moreover, CCN-0.05 can still achieve effective removal of SMX under actual water backgrounds and showed selective degradation on sulfonamides.
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Shang Kefeng,Feng Xi,Wang Yongxin
MgCoFe layered double oxides (MgCoFe-LDO) were fabricated to activate peroxymonosulfate (PMS) for degradation of sulfamethoxazole (SMX), and the highly efficient degradation of SMX revealed an excellent catalytic activity of Mg 2 Co 1 Fe 1 -LDO for PMS under different pH values and water matrix. Scanning electron microscope analysis indicated the catalyst has a typical “flower-like” structure, and the X-ray powder diffraction analyses proved that the main crystal phase of Mg 2 Co 1 Fe 1 -LDO is CoFe 2 O 4 and Mg 1−x Fe x O, which is responsible for the good catalytic activity of Mg 2 Co 1 Fe 1 -LDO. The radical scavenging experiments confirmed that 1 O 2 , \({\text{SO}}_{4}^{\cdot - }\) , OH and \({\text{O}}_{2}^{\cdot - }\) were involved in the degradation of SMX, but 1 O 2 and \({\text{SO}}_{4}^{\cdot - }\) played the dominant roles. According to the X-ray photoelectron spectroscopy (XPS) of Mg 2 Co 1 Fe 1 -LDO catalyst, it was referred that the species including CoOH + , CoO + , Fe 3+ , FeOH 2+ , Fe 2+ , etc. involve in the activation process of PMS. Moreover, the possible degradation pathways of SMX were proposed according to the detected intermediates including N-hydroxy sulfamethoxazole, 3-amino-5-methylisoxazole from LC–MS analysis, and the toxicity analysis via Toxicity Estimation Software Tool software shows that most of the degradation products of SMX have lower toxicity than SMX. Graphical Abstract
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WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 6
·1-20
·
IF 3.8
Akbari Mohammad Zahir,Xu Yifeng,Liang Chuanzhou,Lu Zhikun,Shen Siyuan,Peng Lai
This study aimed to accelerate photocatalytic treatment of sulfamethoxazole (SMX) and cefixime (CFM) and alleviate the toxicity of photocatalysis effluents to improve further biodegradability. An efficient and fast reactive photocatalyst (Fe 2 O 3 /ZnO@VC) was synthesized, characterized and applied for photocatalytic removal of the targeted compounds. Results further confirmed the complete removal of SMX (1 mgL -1 ) within 30-min photocatalytic treatment. Acidic condition favored SMX removal due to the formation of negative ions, which were attracted by the surface of the catalyst comprising positive charge in pH values below the point of zero charge. The ideal degradation environment for CFM (1 mgL -1 ) was at neutral pH, and 97.2±0.1% of CFM was degraded over 60-min. A quenching test revealed that superoxide radial ( • O 2 − ) and e − played a major role in the photocatalytic degradation of SMX, while hydroxyl radical ( • OH) showed an identical effect during photocatalytic treatment of CFM. The degradation efficiency of SMX was marginally reduced in synthetic wastewater (SWW) and CFM in tap water (TW) due to the quenching effects of phosphates and carbonates anions in SWW and chloride ions in TW, respectively. As a result of the excellent mineralization properties of the photocatalyst, the photocatalysis effluents were highly detoxified, reaching 93.5±11.8% and 87.0±5.1% for SMX and CFM, respectively. Graphical Abstract
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BIORESOURCE TECHNOLOGY
·
2024
·
IF 9.7
Zhibin Liu,Xuelin Shi,Zihao Yan,Zhirong Sun
In this study, a 3D CoNiO 2 /Co core–shell structure biochar catalyst derived from walnut shell was synthesized by hydrothermal and ion etching methods. The prepared BC@CoNi-600 catalyst exhibited exceptional peroxymonosulfate (PMS) activation. The system achieved 100 % degradation of sulfamethoxazole (SMX). The reactive oxygen species in the BC@CoNi-600/PMS system included SO 4 − , OH, and O 2 − . Density functional theory calculations explored the synergistic effects between nickel–cobalt bimetallic and carbon matrix during PMS activation. The unique 3D core–shell structure of BC@CoNi-600 features an outer nickel–cobalt bimetallic layer with exceptional PMS adsorption capacity, while protecting the zero-valence Co of the inner layer from oxidation. Based on the experimental-data, machine learning modeling mechanism, and information theory, a nonlinear modeling method was proposed. This study utilizes a machine learning approach to investigate the degradation of SMX in complex aquatic environments. This study synthesized a novel biochar-based catalyst for activated PMS and provided unique insights into its environmental applications.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lan Xie,Jiajia Hao,Yinsu Wu,Shengtao Xing
Non-radical activation of peroxymonosulfate (PMS) is a promising technology for removing refractory organic pollutants. However, improving its efficiency is still a challenge due to its ambiguous mechanism. In this work, amorphous MnO X was synthesized through the hydrothermal reaction between KMnO 4 and carbon nanopowder. The characterization results indicate that the hydrothermal temperature had little effect on the structure of the products but affected their surface composition. The sample prepared at 180 °C (MnO X -180) had rich oxygen vacancies and exhibited high activity for sulfamethoxazole (SMX) degradation with PMS. More than 97% of SMX was removed within 30 min by 0.5 g L −1 of MnO X -180 and 1 mmol L −1 of PMS at pH 0 = 6.5. Activated PMS adsorbed on catalyst surface and singlet oxygen ( 1 O 2 ) produced from the non-radical pathway were the active species. Surface Mn 4+ and oxygen vacancies were found to be responsible for the generation of activated PMS and 1 O 2 , respectively. The degradation efficiency of SMX by MnO X -180 increased with decreasing solution pH, which can be attributed to the enhanced production of activated PMS under acidic conditions. The water matrix had little effect on the performance of MnO X -180 due to the non-radical activation mechanism, suggesting its practical application in real water treatment.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yan Chen,Yufan Liu,Huizhen Jin,Xinyue Wang,Guowen Wang,Hongchao Ma,Vadivel Subramaniam,Krishnamoorthy Ramachandran,Xinghui Liu
Antibiotic drugs are biotoxic and difficult to degrade, causing irreversible effects on aquatic environment and human health. The photoelectrocatalytic (PEC) process is regarded as a promising strategy for simultaneously addressing environmental pollution and the energy crisis. Herein, a plum tree-type composite semiconductor photoanode MnOx@Co/NC-x with core-shell heterostructures was constructed to evaluate the PEC activity for sulfamethoxazole (SMX). The synergistic effects of Co nanoparticles, a high content of graphitic N, an open framework, and interfacial structures played a decisive role in improving the PEC activity of the MnOx@Co/NC-x system. The engineered micro-nano structure significantly improved the specific surface area and conductivity of electrode materials, and promoted the diffusion of electrolyte. Among them, MnOx@Co/NC-500 photoanode exhibited the best performance (reached 98.92% in 50 min), cyclic stability and repeatability. The results showed that it was feasible to construct a high-performance heterostructural interface for pollutant treatment based on micro-nano structure regulation and valence band matching.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yuanyuan Zhang,Leiyun Li,Zihan Pan,Yunjie Zhu,Yanan Shao,Yinghui Wang,Kefu Yu
Sulfate radical (SO 4 − ) based advanced oxidation processes are effective for the removal of antibiotics including sulfonamides from freshwater. However, few studies were focused on the degradation of sulfonamides in marine aquaculture water and seawater, as well as the impact of transformation products on seafood such as fishes. In this work, sulfamethoxazole (SMX) was treated with UV/persulfate (UV/PS) system in different water samples. Chloride ions (Cl − ) had an inhibitory effect possibly due to the consumption and mutual quenching of reactive radicals. A slight promotion by bromide ions (Br − ) was observed and should be related not only to the transformation of Br , but also to the properties of the SMX itself. Bicarbonate ions (HCO 3 – ) significantly inhibited degradation as it is a scavenger of SO 4 − and HO in UV/PS. Sulfate ions (SO 4 2− ) showed a negligible impact on SMX degradation. The active sites of SMX were calculated to be the N1 and C7 atoms of the isoxazole ring, as well as the C9, C13 and N3 atoms of the benzene ring. Seven organic transformation products were identified by LC-MS/MS. Bromate (BrO 3 − ) and chloromethane as the potential human carcinogens were not detected from the reaction system of UV/PS with SMX in marine aquaculture water and seawater. Preliminary analysis of toxicity by the EPI Suite model, absorbable organic halogen (AOX) analysis and growth inhibition of Chlorella vulgaris proved that the UV/PS process could be used as a new disinfection method and it is relatively safer than traditional UV/NaClO disinfection.
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