Scientific Reports
·
2023
·Vol. 13
·期 1
·1-14
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IF 4.6
Alishiri Mahsa,Gonbadi Maryam,Narimani Mehdi,Abdollahi Seyyed Amirreza,Shahsavaripour Negin
The contamination of the aquatic environment with antibiotics is among the major and developing problems worldwide. The present study investigates the potential of adsorbent magnetite-chitosan nanoparticles (Fe 3 O 4 /CS NPs) for removing trimethoprim (TMP) and sulfamethoxazole (SMX). For this purpose, Fe 3 O 4 /CS NPs were synthesized by the co-precipitation method, and the adsorbent characteristics were investigated using XRD, SEM, TEM, pH zpc , FTIR, and VSM. The effect of independent variables (pH, sonication time, adsorbent amount, and analyte concentration) on removal performance was modeled and evaluated by Box–Behnken design (BBD). The SEM image of the Fe 3 O 4 /CS adsorbent showed that the adsorbent had a rough and irregular surface. The size of Fe 3 O 4 /CS crystals was about 70 nm. XRD analysis confirmed the purity and absence of impurities in the adsorbent. TEM image analysis showed that the adsorbent had a porous structure, and the particle size was in the range of nanometers. In VSM, the saturation magnetization of Fe 3 O 4 /CS adsorbent was 25 emu g −1 and the magnet could easily separate the adsorbent from the solution. The results revealed that the optimum condition was achieved at a concentration of 22 mg L −1 , a sonication time of 15 min, an adsorbent amount of 0.13 g/100 mL, and a pH of 6. Among different solvents (i.e., ethanol, acetone, nitric acid, and acetonitrile), significant desorption of TMP and SMX was achieved using ethanol. Also, results confirmed that Fe 3 O 4 /CS NPs can be used for up to six adsorption/desorption cycles. In addition, applying the Fe 3 O 4 /CS NPs on real water samples revealed that Fe 3 O 4 /CS NPs could remove TMP and SMX in the 91.23–95.95% range with RSD (n = 3) < 4. Overall, the Fe 3 O 4 /CS NPs exhibit great potential for removing TMP and SMX antibiotics from real water samples.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yiqing Liu,Ting Wang,Zhengjie Chen,Shenglan Liu,Yongsheng Fu
Currently, the research on bisulfite (BS) activation by Mn(II) is very limited probably because of the low catalytic efficiency of Mn(II). Adding ligands to Mn(II)/BS system is likely to improve the BS activation, but the relative information is very rare. Therefore, the effect of nitrilotriacetic acid (NTA) on Mn(II)/BS system was investigated in this work using sulfamethoxazole (SMX) as the target contaminant. The results showed that the addition of NTA enhanced SMX removal in Mn(Ⅱ)/BS system through forming Mn(Ⅱ/III)-NTA complexes driving Mn(III)/Mn(II) cycle and stabilizing Mn(III). Alcohol scavenging experiments and competitive kinetic experiments indicated that sulfate radical (SO 4 •− ) and hydroxyl radical (HO • ) were not the main reactive species in Mn(II)/NTA/BS system. Mn(Ⅲ) was the primary oxidant for SMX elimination in this system and its existence was proved by UV-Vis absorption spectrum of reaction solution. Mn(Ⅱ)/NTA/BS system could greatly degrade SMX in near-neutral conditions, while nearly no SMX removal was observed at pH 3.0. The decrease of dissolved oxygen concentration significantly inhibited BS autocatalytic stage, thus suppressing the removal of SMX. Due to the competitive complexation of HCO 3 − and FA with NTA for Mn(II), their addition in Mn(Ⅱ)/NTA/BS system obviously inhibited SMX degradation . Four intermediates were detected during SMX degradation in Mn(Ⅱ)/NTA/BS system, and the possible SMX transformation pathways were speculated as N-S bond breaking, hydroxylation, amino oxidation and coupling reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shijing Li,Xiangyong Zheng,Huachang Jin,Linbo Qian,Kun Wang,Yi Shen,Min Zhao,Renlan Liu
Peroxymonosulfate(PMS)-based advanced oxidation technologies have rapidly evolved in the past few years with cobalt being one of the most powerful PMS activators, demonstrating considerable potential in environmental pollution control. Using water-soluble sulfonated cobalt(II) phthalocyanine as the precursor, a graphene-based catalyst with a three-dimensional macrostructure containing Co(II) and Co(III) was created through simple freeze-drying and high-temperature calcination herein. The multivalent cobalt effectively improved the reaction rate of material activation PMS to degrade SMX, and the presence of the sp 2 -hybridized carbon lattice accelerated the electron-transfer rate. Through quenching experiments and electron paramagnetic resonance, it was demonstrated that high-valent cobalt-oxo species [Co(IV) = O] were the primary active components of the reaction system, and that the cobalt–nitrogen active components and N vacancy structure in the material were conducive to the formation of high-valent Co(IV) = O species and 1 O 2 . Furthermore, after reusing the manufactured materials 10 times, the reaction system was still able to remove SMX efficiently, allowing for the practical implementation of PMS advanced oxidation technology. Thus, the current study considerably contributes to the investigation of the PMS reaction mechanism of multivalent cobalt-doped graphene catalytic materials.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Wenjun Zhu,Shuai Zhang,Xiaohua Zuo,Xin Li,Xiangyi Deng,Guanghui Wang,Deng Ding,Chunlei Wang,JunTao Yan,Xiaobo Wang
The magnetic CuFeO 2 anchored on nitrogen-doped porous carbon (CuFeO 2 /NC) hybrid catalysts were further synthesized via hydrothermal reaction without the addition of a chemical reductant. The systematic CuFeO 2 /NC with larger specific surface areas (SSAs) and abundant active sites exhibited strong adsorption ability and great catalytic performance towards activating peroxymonosulfate (PMS) for sulfamethoxazole (SMX) removal. It was noted that 18 mg/L SMX was completely removed after 40 min of pre-adsorption and 30 min of oxidative degradation in CuFeO 2 /NC and PMS system. The degradation rate constant ( k ) was calculated by fitting as 0.166 min −1 , being about 7.9 times that in the CuFeO 2 and PMS system (0.021 min −1 ). The SO 4 · - ,·OH, and 1 O 2 as the dominant reactive oxygen species (ROSs) contributed to sulfamethoxazole degradation. The N species, active oxygen and the redox cycles of Cu(Ⅱ)/Cu(Ⅰ) and Fe(Ⅲ)/Fe(Ⅱ) were confirmed to play a vital role in the activation of PMS for the generation of ROSs. Based on the LC-MS analysis, the possible degradation routes of SMX in the PMS activation system by CuFeO 2 /NC were proposed.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2018
·
IF 2.829
Ying Liu,Xiaohui Liu,Guodong Zhang,Tao Ma,Tingqin Du,Yong Yang,Shaoyong Lu,Weiliang Wang
Sulfonamide antibiotics are widely detected in soil, surface water, sediments and drinking water due to their stable nature, which has huge potential risks. In this study, we reclaimed activated carbon with hexadecyl trimethyl ammonium bromide (CTAB) modification (MAC) as the adsorbents to remove aqueous sulfamethazine (SMX) and sulfamethoxazole (SMZ). It was best described by the pseudo second-order model for SMX and SMZ on MAC, where the adsorption rate constant k 2 were 0.0039 and 0.0057 g·mg −1 min −1 , respectively, which indicated that might be the combined effect between in-diffusion, membrane diffusion and surface adsorption. The equilibrium data of SMX and SMZ on MAC were well represented by Freundlich model, while the maximum adsorption capacity of SMX and SMZ by Langmuir model were 16.155 mg g −1 and 17.513 mg g −1 , respectively. SMX and SMZ sorption on MAC revealed pronounced pH dependence. In addition, HA can inhibit the adsorption of SMX and SMZ on MAC. Cd 2+ can promote the sorption ability of SMX on MAC, while Cr 6+ inhibits the adsorption of SMX. Adsorption mechanism of SAs on MAC was clarified, where the hydrogen bonding interaction and π-π EDA interaction contributed most to SAs adsorption. Well, hydrophobic interaction was considered as another adsorption mechanism for SMZ different from SMX, where it might be one of the reasons that the adsorption capacity of SMZ is higher than that of SMX. This study revealed that MAC may be the efficient and practical adsorbent for SAs removal from aqueous environments.
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WATER RESEARCH
·
2018
·
IF 7.051
Yueping Bao,Wen-Da Oh,Teik-Thye Lim,Rong Wang,Richard David Webster,Xiao Hu
In this work, nano-bimetallic Co/Fe oxides with different stoichiometric Co/Fe ratios were prepared using a novel one-step solution combustion method. The nano-bimetallic Co/Fe oxides were used for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation. The stoichiometric efficiencies of the as-prepared nano-bimetallic catalysts were calculated and compared for the first time. The radical generation was identified by electron paramagnetic resonance (EPR) as well as chemical quenching experiments, in which different scavengers were used and compared. The catalytic PMS activation mechanism in the presence of catalyst was examined by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that besides SO 4 • - and •OH, •OOH was also detected in the PMS/CoFeO 2.5 system. Meanwhile, in addition to the previously proposed radical oxidation pathway, the results showed that SMX degradation also involved a non-radical oxidation, which could be verified by the degradation experiment without catalyst as well as the detection of 1 O 2 . In the PMS activation process, cobalt functioned as the active site on CoFeO 2.5 while Fe oxide functioned as the adsorption site. The electron transfer mechanism was proposed based on the XPS and metal leaching results. Additionally, via the detection of transformation products , different SMX transformation pathways involving nitration, hydroxylation and hydrolysis in the PMS/CoFeO 2.5 system were proposed.
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CHEMICAL ENGINEERING JOURNAL
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2018
·
IF 6.735
Yueping Bao,Teik-Thye Lim,Rong Wang,Richard David Webster,Xiao Hu
In this study, a novel CoFe 2 O 4 nanocatalyst impregnated Al 2 O 3 ceramic membrane was prepared via a urea-assisted one-step combustion method. The catalytic membrane was characterized by field emission scanning electron microscopy (FESEM) with energy dispersive X-Ray analysis (EDX) and applied for the catalytic degradation of sulfamethoxazole (SMX) via peroxymonosulfate (PMS) activation under a dead-end membrane filtration mode for the first time. Results indicate that CoFe 2 O 4 could be impregnated into the macropores throughout the whole Al 2 O 3 ceramic membrane via this method and the CoFe 2 O 4 loading amount could be controlled by the multiple impregnation cycles. The membrane filtration operation mode significantly enhances the accessibility of the catalytic active sites to PMS and SMX in microreactor environment and thus the CoFe 2 O 4 impregnated membrane displays excellent catalytic activity for the SMX degradation. The pure water permeability flux can maintain at ∼3000 L m −2 h −1 bar −1 (LMHB) with the catalyst loading amount of 0.015 g/g Al 2 O 3 . In the membrane filtration system, the removal rate of SMX with the initial concentration of 10 mg L −1 can achieve to ∼98%, 70% and 40% with the residence time of 90, 36 and 18 s. The catalytic membrane shows a great tolerance at wide pH range (3–11), the existence of humic acid and anions. Meanwhile, the membrane shows self-cleaning property by retaining >90% of initial flux after 3 treatment cycles. Electron paramagnetic resonance (EPR) and radical quenching experiments indicate that both sulfate radical and hydroxyl radical are generated and sulfate radical is the dominant active species in the process.
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ENVIRONMENTAL TOXICOLOGY AND PHARMACOLOGY
·
2018
·
IF 2.776
Chen Zhou,Huiqing Wang,Youbin Si,Kang Wu,Amina Yousaf
The ability of anthraquinone-2,6-disulfonate (AQDS) and riboflavin to enhance the sulfamethoxazole (SMX) degradation coupled with the Fe(III) reduction by Shewanella oneidensis MR-1 was investigated. The results indicated that the SMX degradation rate was 38.5% with an initial SMX concentration at 0.04 mM. For the overall performance of AQDS and riboflavin mediated SMX degradation and iron reduction, the SMX degradation rate was gradually increased with the enhancement of iron reduction. Riboflavin had a stronger enhancement on SMX degradation and iron reduction than AQDS, but the enhancement was not positively correlated with electron shuttles concentration. A quantitative characterization of the electron transfer capacity (ETC) of the electron shuttles showed that the ETC was higher for riboflavin than AQDS. The S. oneidensis MR-1 16S rRNA gene copies results indicated that electron shuttles had a positive effect on the microbial activity of S. oneidensis MR-1. The LC MS result indicated that the products of the SMX biodegradation were 3-amino-5-methylisoxazole and 4-aminobenzenesulfonic acid, which suggested that the SMX biodegradation was caused by S N bond cleavage. This study indicates that the biochemical mechanisms play a vital role in SMX transformation and Fe(II) generation in this system.
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JOURNAL OF CHROMATOGRAPHY A
·
2015
·
IF 4.169
Yuan Xiao,Jialiang Guo,Danni Ran,Qianqian Duan,Jacques Crommen,Zhengjin Jiang
A facile and efficient “one-pot” copolymerization strategy was used for the preparation of sulfonamide drug (SA) functionalized monolithic columns. Two novel SA-immobilized methacrylate monolithic columns, i.e. poly(GMA-SMX- co -EDMA) and poly(GMA-SAA- co -EDMA) were prepared by one-pot in situ copolymerization of the drug ligand (sulfamethoxazole (SMX) or sulfanilamide (SAA)), the monomer (glycidyl methacrylate, GMA) and the cross-linker (ethylene dimethacrylate, EDMA) within 100 μm i.d. capillaries under optimized polymerization conditions. The physicochemical properties and column performance of the fabricated monolithic columns were characterized by elemental analysis, scanning electron microscopy and micro-HPLC. Satisfactory column permeability, efficiency and separation performance were obtained on the optimized poly(GMA-SMX- co -EDMA) monolithic column for small molecules, such as a standard test mixture and eight aromatic ketones. Notably, it was found that the poly(GMA-SMX- co -EDMA) monolith showed a selective affinity to trypsin, while the poly(GMA-SAA- co -EDMA) monolith containing sulfanilamide did not exhibit such affinity at all. This research not only provides a novel monolith for the selective isolation and purification of trypsin, but it also offers the possibility to easily prepare novel drug functionalized methacrylate monoliths through a one-pot copolymerization strategy.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xiaoxue Pan,Qiyang Liu,Jingjing Jiang,Xingyue Fang,Yingying Liu,Jinli Qiu,Xuesheng Zhang
Burgeoning oxidation technology based on peracetic acid (PAA) has been widely used to treat organic pollutants, and the development of efficient catalytic materials is a vital theme. In this study, a novel catalyst FeCo@NC was designed to degrade sulfamethoxazole (SMX), a typical sulfonamide antibiotic, which not only owned excellent activation performance of PAA, but also presented superior recycling performance and stability. Ten μM of SMX were nearly completely removed within 90 min under the conditions of 25 °C, pH at 7.0, 0.5 g/L catalyst, and 100 μM of initial PAA. FeCo@NC/PAA technique possessed a satisfactory degradation performance on SMX in a wide pH range, and even in the presence of a variety of anions and humic acids. The 90-min degradation rate of SMX in FeCo@NC/PAA system remained above 70 % after 4 cycles. Metal ion leaching data together with the X-ray diffraction (XRD) results confirmed the reusability and stability of this material. Superoxide and organic radicals eliminated SMX via the bond cleavage of S–C or S–N, hydroxylation and coupling reaction to yield 11 intermediates. The S–N bond cleavage was an eco-friendly route. This study provides a reference for the design of effective catalysts and their application in the treatment of refractory organic pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shuang Wu,Yangli Cui,Lan Liang,Wenjie Gao,Zhen Yu,Zhanjun Cheng,Beibei Yan,Guanyi Chen,Ning Li
Heterogeneous catalyst reuse and the effectiveness of hydrogen peroxide (H 2 O 2 )-based advanced oxidation processes under near-neutral conditions remain an obstacle in wastewater remediation. Herein, we put forward a versatile catalytic membrane with Cu-doped MnO active layer anchoring on the polydopamine-modified electrospinning polyvinylidene fluoride (PDA@PVDF) base. The Cu-MnO@PDA@PVDF membrane was conferred admirable sulfamethoxazole (SMX) reduction (over 90% within 90 min) and clogging alleviation (relative flux recovery to 0.98) capabilities via in situ H 2 O 2 activation at pH 8, which was slightly affected by actual water background. Electron paramagnetic resonance (EPR) and trapping tests unveiled the joint contribution of • OH, O 2 •− and 1 O 2 , with • OH exerting the supreme role in SMX oxidation. The inherent characteristics of dual Mn-Cu centers on the membrane surface for facilitation of electron transfer, H 2 O 2 adsorption and barrierless dissociation to • OH were further elucidated by electrochemical measurements and density functional theory (DFT) computation. Comprehensively, this study proposes a facile procedure and insights into engineering catalytic membrane coupled H 2 O 2 strategy for refractory organic treatment at ambient conditions.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yali Song,Ziyan Li,Cairong Yang,Xiaoyu Wen,Long Huang,Xiaojing Zhang,Yongpeng Ma,Qiong Wang,Hongzhong Zhang
To improve the generation of main active substances (·O 2 – and h + ) in sulfamethoxazole (SMX) photocatalytic processes by g–C 3 N 4 , graphitic carbon nitride/perylene diimide (g–C 3 N 4 /PDI, CNPDI) organic photocatalyst with Z–scheme heterojunction was synthesized. Simultaneously, the in–situ self–assembled PDI was realized by introducing short straight–chain alkanes containing terminal carboxylic acid groups at the imide position of PDI molecule and regulating the pH value of the reaction system. g–C 3 N 4 and PDI successfully combined via the formation of –O C–NH– during the preparation process. The π–π interaction between them was conducive to the charge migration at the heterogeneous interface. The addition of PDI in g–C 3 N 4 significantly improved the absorption ability of visible light and facilitated the transportation of photogenerated carriers, leading to enhanced photocatalytic properties. When 2 mg of PDI combined with 500 mg of g–C 3 N 4 , the obtained CNPDI–2 demonstrated the optimal degradation rate for SMX. When reacted for 120 min under visible light, the SMX photodegradation rate by CNPDI–2 was up to 96.3 % because more ·O 2 – and h + generated and participated in the reaction process. The corresponding pseudo–first–order kinetic constant (0.0281 min –1 ) in CNPDI–2 photocatalytic system was 2.4 and 51 times than that in g–C 3 N 4 system (0.0105 min –1 ) and PDI system (0.0005 min –1 ), respectively. Additionally, CNPDI–2 demonstrated the commendable stability, which was suitable for SMX removal in water environment.
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