SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Fan Wu,Xueyu Nie,Yulun Nie,Chu Dai,Xike Tian
As reported, PMS can be activated and decomposed into different reactive oxygen species such as 1 O 2 , • OH and SO 4 •- , besides, coupling of non-radical (PMS direct oxidation) and radical (SO 4 •- ) process could enhance the utilization efficiency of PMS. In this study, we proposed another strategy of 1 O 2 -based non-radical and • OH-based radical process using layered double hydrotalcite (MgAl-LDH and MgAlCu-LDH) to regulate the degradation, transformation and even mineralization of sulfamethoxazole. Compared with PMS direct oxidation , SMX removal efficiency was increased from 41.8% to 71.7% by 1 O 2 . However, there was almost no real degradation or mineralization since the ionization intermediates including C 10 H 12 N 3 O 4 S and C 7 H 9 N 3 O 5 S accumulated with reaction time according to DFT and LC-MSMS analysis. In comparison, 100% of SMX degradation was obtained via coupling 1 O 2 and • OH-radical process, in which the mineralization efficiency reached to 24.8%. Importantly, the above-mentioned intermediates of SMX were not detected and their accumulation were also significantly inhibited. Moreover, SMX degradation behavior and kinetics could be manipulated via direct oxidation , 1 O 2 and then • OH step by step, which was beneficial to enhance the PMS utilization efficiency. Finally, based on the results of zeta potential of MgAlCu-LDH, effect of solution pH on SMX degradation, the interfacial PMS activation process was responsible to regulate non-radical and radical process.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jianbiao Peng,Yu Chang,Lei Xu,Yakun Zhang,Tian Wang,Xinyang Wang,Haijin Liu,Guangxuan Yan,Shixiang Gao,Dexin Liu,Zhiguo Cao
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have shown great potential for recalcitrant contaminants removal in wastewater treatment. Herein, we report the efficient activation of PMS by bimetallic oxides (cobalt and copper) co-doped graphitic carbon nitride (Co–Cu@g-C 3 N 4 ) for removal of sulfamethoxazole (SMX). The morphology and chemical composition of the fresh and used Co–Cu@g-C 3 N 4 were characterized by TEM, SEM, XRD, BET, and XPS. Nearly complete removal of SMX (50 mg/L) was observed in the presence of 50 mg/L Co–Cu@g-C 3 N 4 , 0.5 mmol/L PMS within 20 min at neutral pH with a degradation rate of 0.137 min −1 . Moreover, the Co–Cu@g-C 3 N 4 catalyst enabled more than 90 % removal of various typical pollutants within 20 min, including sulfapyridine, rhodamine B, acridine red, and malachite green, with rate constants of 0.083, 0.130, 0.096, and 0.160 min −1 , respectively. Quenching experiments and electron paramagnetic resonance (EPR) analysis demonstrated that sulfate radical (SO 4 − ) and singlet oxygen ( 1 O 2 ) were collectively responsible for SMX degradation. The efficient activation of PMS by Co–Cu@g-C 3 N 4 was ascribed to the continuous conversion of Co(Ⅲ) to Co(Ⅱ) and Cu(I) to Cu(ⅠI), and the presence of oxygen vacancy (O V ) on the catalyst. The Co–Cu@g-C 3 N 4 /PMS system exhibited superior durability and maintained high efficiency in real water samples. Finally, theoretical calculations of Fukui index were performed to determine the possible degradation pathways of SMX, and the ecotoxicity of the degradation products was evaluated by the ECOSAR program. This study significantly advances the understanding of the reaction between PMS and bimetallic oxides catalysts, as well facilitates the development and application of PMS-based AOPs in wastewater treatment.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Yating Yan,Huayu Zhang,Wei Wang,Wenchao Li,Yueping Ren,Xiufen Li
Developing highly efficient, reusable, non-toxic and low-cost catalysts is of great importance for persulfate-based advanced oxidation processes (AOPs). In this work, ferrocene was mixed into paraffin to prepare a candle, and the iron-containing candle soots were collected and heated at 500 °C~900 °C under N 2 atmosphere for 1 h to prepare magnetically recyclable Fe 0 /Fe 3 O 4 @porous carbon (Fe 0 /Fe 3 O 4 @PC) catalysts. The Fe 0 /Fe 3 O 4 @PC-700 obtained after pyrolysis at 700 °C exhibited the best catalytic activity for sulfamethoxazole (SMX) degradation. 10 mg/L SMX could be completely degraded within 10 min by 0.2 g/L of Fe 0 /Fe 3 O 4 @PC-700 and 0.5 mM PMS at pH 5.0. The carbon shell effectively inhibited the Fe leaching of Fe 0 /Fe 3 O 4 @PC-700, and 99.73% of Fe was retained after five consecutive cycles. In the Fe 0 /Fe 3 O 4 @PC-700/PMS system, SMX was degraded through the sulfate radical (SO 4 · ¯ ), hydroxyl radical (·OH), superoxide radical (O 2 · ¯ ) dominated radical pathway, and the singlet oxygen ( 1 O 2 ) dominated non-radical pathway. The coexisting inorganic ions and natural organic matters (NOM) in actual water inhibited the degradation of SMX. Finally, four possible degradation pathways were proposed based on the degradation intermediates of SMX. This work provides a facile heat treatment of iron-containing candle soots strategy to prepare the metal@carbon catalysts for PMS-based AOP.
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REACTIVE & FUNCTIONAL POLYMERS
·
2020
·
IF 3.333
Wenming Yang,Yujie Qing,Yunfei Cao,Yu Luan,Yi Lu,Tianshu Liu,Wanzhen Xu,Weihong Huang,Tianzhu Li,Xiaoni Ni
In this study, a novel kind of pH-responsive, magnetic and core-shell structured molecularly imprinted polymer (pH-MMIPs) was synthesized for the selective recognition of sulfamethoxazole (SMX). It was synthesized by way of surface imprinting and free radical polymerization . The composition and structure of pH-MMIPs has magnetic nanoparticles as its core, a thin imprinted polymer layer as its shell using 2-(Dimethylamino) ethyl methacrylate and 4-vinylphenylbronic acid as the pH-sensitive monomers , and SMX as template molecule. Interestingly, the pH-MMIPs could control the capture/release process in the selective recognition and detection of SMX by changing the pH value. Evaluation of the property of pH-MMIPs through series of adsorption experiments showed that it has an adsorption capacity of 25.41 mg·g −1 with a very rapid speed of magnetic separation. Additionally, it was successfully applied to selectively detect SMX in real milk samples, and the recoveries was in ranges of 89.7% and 98.2%. This study provides a new method and idea for the selective separation of SMX residue in food using molecularly imprinted polymers with pH- response and identification.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 29
·期 4
·6237-6250
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IF 4.223
Chen Xi,Lin Hai,Dong Yingbo,Li Bing,Yin Tingting,Liu Chenjing
The complex mixtures of antibiotics and heavy metals are commonly existed in livestock and poultry breeding wastewater. Effective and simultaneous removal of these toxic compounds by microorganisms, especially single strains, remains a considerable challenge. In this study, a novel functional strain SDB4, isolated from duck manure and identified as Bacillus sp., has been shown to possess high removal capabilities for both sulfamethoxazole (SMX) and Zn 2+ . The maximum removal efficiency achieved 73.97% for SMX and 84.06% for Zn 2+ within 48 h in the single pollution system. It has great potential for eliminating SMX along with Zn 2+ , 78.45% of SMX and 52.91% of Zn 2+ were removed in the 20 mg·L -1 SMX and 100 mg·L -1 Zn 2+ binary system. Furthermore, the SMX-biotransformation capability of SDB4 was enhanced at low concentrations of Zn 2+ (below 100 mg·L -1 ). The SMX biotransformation and Zn 2+ adsorption data fitted well with the pseudo-first-order kinetic model, indicating that the two pollutants were in accordance with the same removal rule. N 4 -acetyl-SMX was identified as the main stable transformation product during SMX removal. FTIR analyses revealed that OH, NH 2 , C=O, C-N/N-H, and C-O-C played major roles in the adsorption of Zn 2+ . Our study of the dually functioning strain SDB4 provides a potential application for the simultaneous biological removal of antibiotics and heavy metals.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2016
·
IF 3.299
Jie Xu,Weiying Xu,Dongsheng Wang,Guoqing Sang,Xiaoshuai Yang
The removals of humic acid (HA) and a kind of antibiotic compound by enhanced coagulation (EC) employing various Al-based coagulants with, and without MIEX resin pre-treatment were systematically investigated in this study. A range of techniques were used to evaluate the purification behaviors and mechanisms of the coagulation and MIEX adsorption processes . The experimental results indicated that sufficient dose of Al-based coagulants removed 60–70% of HA, while traditional Al 2 (SO 4 ) 3 (AS) coagulant with low dose of 1.0–5.0 mg/L coupled with MIEX contributed to a removal rate of 85%. For sole coagulation, Al 13 ([Al 13 O 4 (OH) 24 (H 2 O) 12 ] 7+ ) only removed 11% to <23% of SMX, while AS and polyaluminum chloride (PACl) contributed to comparable removal of about 40%, indicating charge neutralization was not the major mechanism in SMX removal. The SMX removal could be improved to 68–78% by MIEX pre-treatment. Dynamic floc sizes during coagulation processes were studied using a laser diffraction particle sizing device. The results demonstrated Al 13 led to the smallest flocs, while the adsorption and sweep mechanisms in AS and PACl coagulation processes resulted in larger aggregates. Besides, the pretreatment of MIEX could evidently decrease the floc sizes for all the coagulants.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Wondimeneh Dubale Adane,Bhagwan Singh Chandravanshi,Merid Tessema
In this study, we have developed a novel, hypersensitive, and ultraselective electrochemical sensor containing thermally annealed gold–silver alloy nanoporous matrices (TA-Au-Ag-ANpM) integrated with f -MWCNTs-CPE and poly( l -serine) nanocomposites for the simultaneous detection of sulfathiazole (SFT) and sulfamethoxazole (SFM) residues in honey, beef, and egg samples. TA-Au-Ag-ANpM/ f -MWCNTs-CPE/poly( l -serine) was characterized using an extensive array of analytical (UV–Vis, FT-IR, XRD , SEM , and EDX), and electrochemical (EIS, CV and SWV) techniques. It exhibited outstanding performance over a wide linear range, from 4.0 pM to 490 μM for SFT and 4.0 pM to 520 μM for SFM, with picomolar detection and quantification limits (0.53 pM and 1.75 pM for SFT, 0.41 pM and 1.35 pM for SFM, respectively). The sensor demonstrated exceptional repeatability, reproducibility, and anti-interference capability, with percentage recovery of 95.6–102.4% in food samples and RSD below 5%. Therefore, the developed sensor is an ideal tool to address the current antibiotic residue crisis in food sources.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Chen Wang,Yubei Liu,Mingjie Huang,Wei Xiang,Tao Zhou,Xiaohui Wu,Juan Mao
It was demonstrated in this study that appropriate concentrations of oxalate (Ox) would lead to greatly accelerated electro-generation of Fe 2+ but obviously lower power consumption in the Fered-Fenton system. Depending on the Ti electrode with pristine TiO 2 layer, effects of important parameters on the SMX degradation were investigated in the Fered-Fenton-Ox system. It was found that the heterogeneous interfacial electrochemically reduction of Fe III was critical in the Fered-Fenton-Ox system relying on the surface hydroxyl bonding Fe III -Ox and formation of Fe O Ti bonds. A heterogeneous-homogeneous reaction mechanism was therefore proposed. It included the heterogeneous interfacial electrochemical generation of Fe II -Ox and the heterogeneous-homogenous Fenton oxidation of pollutants. The promotional role of Ox would be also homogenous and heterogeneous, i.e. maintaining ferric at higher pH and forming specific Fe III -Ox complex as well as accelerating the solid-liquid interfacial heterogeneous iron cycle. Furthermore, a continuous-flow pilot study was conducted in treating a printing and dyeing industrial wastewater. As compared to conventional Fenton and Fered-Fenton systems, the Fered-Fenton-Ox system could achieve more efficient COD removal with a relative low cost/△COD, suggesting great advantages in its practical applications for treating real industrial complex wastewaters.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
·
IF 5.589
Xiaojing Zhang,Zhao Chen,Yongpeng Ma,Nan Zhang,Denghui Wei,Hongli Zhang,Hongzhong Zhang
Considering the inevitable release of antibiotics and nanoparticles (NPs) into the nitrogen containing wastewater, the combined impact of CuO NPs and sulfamethoxazole (SMX) antibiotic on partial nitrification (PN) process was investigated in four identical reactors. Results showed that the bioactivity of the aerobic ammonia-oxidizing bacteria (AOB) decreased by half after they were exposed to the combination of CuO NPs and SMX for short-term; however, there was no obvious variation in the bioactivity of AOB when they were exposed to either CuO NPs or SMX. During long-term exposure, the ammonia removal efficiency (ARE) of CuO NPs improved whereas that of SMX decreased, while the combination of CuO NPs and SMX significantly decreased ARE from 62.9% (in control) to 38.2% and had an unsatisfactory self-recovery performance. The combination of CuO NPs and SMX significantly changed the composition of microbial community, decreased the abundance of AOB, and significantly suppressed PN process. Reegarding the resistance genes, the CuO NPs-SMX combination did not improve the expression of copA , cusA , sul1 and sul2 ; however, it significantly induced the expression of sul3 and sulA .
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Yingjian Yu,Xiaolong Chen,Dan Zheng,Yulong Li,Zhuqi Chen,Rong Chen,Lie Yang
In this study, a novel iron-zinc bimetal-loaded sludge biochar-based biochar (Fe-Zn@SBC) was prepared for efficient removal of sulfamethoxazole (SMX) from aquatic environments through the activation of periodate (Pl). The addition of bimetals resulted in a unique honeycomb-like microstructure within the biochar, significantly affecting its pore distribution, functional group intensity, and defect characteristics. The Fe-Zn@SBC catalyst demonstrated exceptional performance in activating PI across a wide range of pH conditions and exhibited robustness against interference from prevalent contaminants in water bodies. Quenching experiments, electron paramagnetic resonance (EPR) analysis, and electrochemical assessments indicated that the degradation of SMX primarily occurs through a radical pathway driven by superoxide radicals, alongside a non-radical pathway facilitated by electron transfer. The synergistic interaction between Fe-Zn@SBC and PI enhanced the degradation of SMX into various small molecular intermediates, thereby contributing to the safety of aquatic ecosystems. This research presents an innovative modification strategy for sludge biochar, providing an effective and environmentally sustainable approach to mitigating pollution from pharmaceutical active compounds (PhACs) in aquatic systems.
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RSC Advances
·
2025
·Vol. 15
·期 7
·5042-5059
·
IF 4.6
Irfan Ijaz,Aysha Bukhari,Ammara Nazir,Ezaz Gilani,Hina Zain,Attia Shaheen,Mohammed Rafi Shaik,Mujeeb Khan,Jilani P. Shaik
The simultaneous removal of antibiotics and heavy metal ions is of utmost importance because of their hazardous effects on the environment and humans. For the adsorption of sulfamethoxazole (SMX) and neodymium (Nd3+) in mono- and binary contaminant systems (SMX–Nd3+ and Nd3+–SMX), a novel composite was designed using sulfated fucan (FuS), MXenes, and α-aminophosphonates (AMPs) in this study. As far as we know, the concurrent adsorption of SMX and Nd3+ employing materials made of MXenes, FuS, and AMPs with this specific structure has not yet been reported. At 318 K, the FuS@MXene@AMP adsorbent demonstrated excellent adsorption capacities of 448.91 and 255.78 mg g−1 for SMX and Nd3+, respectively. The pseudo-first-order (PSO) kinetic model was the most appropriate for depicting the adsorption of SMX and Nd3+ among all the tested kinetic models. The adsorption of SMX and Nd3+ is better described by the Langmuir isotherm model with a higher value of adsorption capacity and R2. The simultaneous presence of Nd3+ and SMX promoted mutual sorption between the antibiotic and metal ions in the binary systems. The results of FTIR and XPS studies indicated that the removal mechanisms were primarily due to hydrogen bonding, complexation, electrostatic interaction, and π–π interaction.
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CHEMOSPHERE
·
2022
·
IF 8.943
Cuiwen Tan,Jiapeng Zhong,Xiaoshan Zheng,Qianxin Zhang,Ping Chen,Mingchang Zhan,Haijin Liu,Wenying Lv,Guoguang Liu
Effective photoexcitation and carrier migration are the essential aspects to strengthen semiconductor-engaged redox reaction. Herein, a three-dimensional thin-wall hollow porous cystic-like g-C 3 N 4 (HPCN) with curved layer edge was successfully fabricated via a non-template thermal-condensation strategy. The construction of unique distorted structure can evoke the hard-to-activate n→π* electronic transition to some extent, broadening the absorption spectrum to 800 nm. And benefiting from the multiple reflections of incident light, the effective photoactivation can be further achieved. Moreover, the thin-wall porous framework can shorten the diffusion distance and accelerate migration of photogenerated charge, favouring interfacial redox reactions. The optimized HPCN 1.0 demonstrated an excellent photocatalytic degradation of SMX under blue-LED light irradiation, which was dramatically superior to that of pristine g-C 3 N 4 (CN, 11.4 times). Ultimately, in consideration of reactions under several influencing factors with four different water samples, we demonstrated that the HPCN photocatalyst could be utilized far more productively for the elimination of SMX under real-world aqueous conditions. This work provides a straightforward approach for the removal of SMX and has immense potential to contribute to global scale environmental remediation.
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