WATER AIR AND SOIL POLLUTION
·
2026
·Vol. 237
·期 6
·391
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IF 3
Zhang Xilong,Tang Zihan,Liu Fei,Hong Xiuping,Zhang Yingying,Fang Ting,Fan Rongjian,Wang Xin
Combined pollution by antibiotics and microplastics poses a significant threat to aquatic ecosystems and human health. Polystyrene (PS), a typical microplastic widely detected in aquatic environments, interacts with the sulfonamide antibiotic sulfathiazole (STZ) and thereby impacts wastewater treatment processes. In this study, a novel magnetic biochar (MBC) was synthesized via co-precipitation. Its performance in removing STZ in the presence of PS was systematically evaluated using experimental and theoretical calculation methods. The MBC exhibited excellent superparamagnetism (saturation magnetization: 11 emu·g −1 ) and a high specific surface area (703 m 2 /g). In a single-pollutant system (STZ only), the MBC achieved an STZ adsorption capacity of 39.3 mg·g −1 . In contrast, the coexistence of PS in the STZ-containing system exerted a promotional effect, increasing the STZ adsorption capacity to 42.5 mg∙g −1 (removal rate > 98%), with optimal performance under neutral conditions (pH 5.00–7.00). Notably, the MBC also maintained high efficiency in PS removal (up to 98%) while eliminating STZ. Kinetic analysis revealed that STZ adsorption in the single-pollutant system relied on hydrogen bonding and π-π conjugation. However, in the co-pollutant system (PS + STZ), PS formed complexes with STZ. These complexes anchored to the hydrophobic regions of the MBC, while the polar groups of STZ bound to the polar sites of the MBC, further enhancing the stability of PS-MBC binding. This is the first study to clarify that PS promotes STZ adsorption on MBC through complex formation, while also enabling efficient PS removal. It bridges the existing knowledge gap in the mechanism of co-pollutant removal and provides a feasible strategy for the synergistic elimination of antibiotics and microplastics.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhangsong Jiang,Xiangfeng Huang,Qiaofeng Wu,Mi Li,Qili Xie,Zuwen Liu,Xiaoming Zou
Although microplastics (MPs) and sulfonamides (SAs) are emerging aquatic pollutants, the structural effects of SAs following their adsorption on MPs and underlying mechanisms of the same remain unelucidated. In this study, the characteristics of the adsorption of 10 SAs on polyamide (PA) were analyzed, and significant structural effects of the former were observed at different pH values (P < 0.01). The highest adsorption distribution coefficient ( K d ) was ∼7.83–43.57 times the lowest one. The key processes and micromechanisms of SA adsorption on PA were revealed using the quantitative structure–activity relationship model and partial least squares structural equation model (PLS-SEM). The results suggest that both the octanol–water partition coefficients ( K ow ) of SAs and the valid adsorption energies ( E ad-v ) between PA and SAs are vital in the observed structural effects of SAs. Furthermore, the density functional theory results demonstrated that during the adsorption of SAs on PA, the different adsorption energies were engendered by equilibrium configurations and interactions, such as hydrophobic, hydrogen bond (H-bond), van der Waals, and electrostatic interactions. Moreover, the developed PLS-SEM models revealed that during the adsorption of cationic (PA–SA + ) and anionic (PA–SA − ) SAs, the structural effects were partially driven by the electrostatic interactions. Conversely, the structural effects of neutral SA (SA 0 ) adsorption on PA were partially due to H-bond interactions. Overall, we pioneered a theoretical basis to understand the structural effects of SAs following their adsorption on MPs.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yulong Yuan,Minghua Nie,Caixia Yan,Leliang Wu,Wenbo Dong,Mingjun Ding,Peng Wang
This study investigated for the first time the potential of the novel combination of peroxymonosulfate (PMS) and carbonate (CO 3 2− ) toward bisphenol S (BPS) under solar light irradiation. Compared with the Na 2 CO 3 /PMS and solar/PMS system, the solar/Na 2 CO 3 /PMS system significantly reduces the time required for the degradation of BPS. The excellent removal performance is possible due to the synergistic effect between enhanced light absorption and PMS activation, which accelerated the decomposition of PMS to generate more reactive oxygen species. Scavenging tests and electron paramagnetic resonance analysis revealed that the singlet oxygen ( 1 O 2 ) was the dominant oxidant formed and contributed to BPS elimination with a small proportion of superoxide anion radical (O 2 •– ), rather than sulfate radical (SO 4 •− ) and hydroxyl radical (HO•). The addition of Cl − could promote the degradation of BPS, but the addition of HA and a higher HCO 3 − concentration inhibited this process. The presence of SO 4 2− and NO 3 − slightly promote the degradation of BPS. Besides, the solar/Na 2 CO 3 /PMS system represented significant degradation efficiency in a wide initial pH range (5.02–10.96). Such a system is favorable for the application in actual water matrices such as domestic wastewater, river water, lake water, and tap water. Meanwhile, based on the intermediates identified, the possible degradation pathways of BPS were proposed. In addition, most of the degradation intermediates of BPS were less toxic to different organisms than the parent compound. Moreover, the highly efficient degradation of several typical organic contaminants was also achieved using the solar/Na 2 CO 3 /PMS system under simulated and natural solar light irradiation. This study provides a novel idea and demonstrates the great potential for the elimination of organic pollutants in water.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Rongfang Yan,Zhenhua Wen,Xuelian Hu,Wenxiu Wang,He Meng,Yang Song,Shuo Wang,Yiwei Tang
Various types of fluorescent nanoparticles have been proposed for the detection of veterinary drug residues in food. However, structure-induced fluorescence nanoparticles with biodegradability and the capacity to conjugate with molecular recognition elements are lacking. Here, a biodegradable tryptophan-phenylalanine dipeptide-based nanomaterial was assembled and modified with a sulfadimethoxine aptamer ( [email protected] ). Then, a novel and efficient fluorescence sensing strategy, based on [email protected] and BHQ1-labeled single-stranded DNA ( [email protected] ), was developed for sulfadimethoxine determination. Under optimal conditions, the fluorescence was linear in the range of 0–200 ng/mL sulfadimethoxine with a detection limit of 1.47 ng/mL (S/N = 3). Satisfactory recoveries of standard additions were found between 92.88 % and 114.15 % for water and milk samples with a relative standard deviation less than 5.0 %, suggesting that the proposed fluorescence sensing strategy can be applied reliably in sulfadimethoxine analysis of liquid foods.
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CHEMOSPHERE
·
2022
·
IF 8.943
Xuqian Wang,Zhimei He,Yi Xie,Yongkui Zhang,Yabo Wang
Peroxymonosulfate (PMS) activation-based advanced oxidation technology possesses great potential for antibiotic-containing wastewater treatment . Herein, we developed an iron phosphide/carbon composite and verified its capability and superiority towards a model antibiotic pollutant (sulfathiazole, STZ) degradation through PMS activation. Benefiting from the chelating ability of phytic acid (PA) with metal ions and its abundance on phosphorous element, a PA-Fe 3+ complex was firstly formed and then served as sole precursor for iron phosphide formation by anoxic pyrolysis . Well crystalized FeP particle were found loading on the simultaneously formed thin layer carbon structure. Catalytic activity evaluation showed that FeP/carbon composite could remove over 99% of STZ (20 mg L −1 ) in 20 min adsorption and 30 min catalysis process under the reaction conditions of catalyst dosage 0.2 g L −1 , PMS loading 0.15 g L −1 . A pseudo-first-order reaction rate constant of 0.2193 min −1 was obtained, which was among the highest compared with reported studies. Further investigations indicated that the developed FeP/carbon composite worked well in a wide solution pH range of 3–9. Reaction mechanism study showed that reactive species of SO 4 − • and 1 O 2 generated from PMS activation played major roles for STZ degradation. Based on liquid chromatography-mass spectroscopy (LC-MS) analysis, a few STZ degradation intermediate products were identified, which facilitated the proposal of STZ degradation pathways. The possible ecological risk of STZ and related degradation intermediates were also considered by toxicity assessment using the Ecological Structure Activity Relationships (ECOSAR) Class Program. The obtained acute and chronic toxicity values implied the relatively low ecological risk of FeP/carbon-PMS reaction system for STZ treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Meng Xie,Mingya Yao,Shiyong Zhang,Lingshuai Kong,Lingxi Zhao,Jinhua Zhan,Ru-Song Zhao
Carbon-based single-atom cobalt catalysts exhibit high catalytic activity for the removal of novel pollutants in advanced oxidation processes. Here, atomically dispersed Co species with five-coordinated nitrogen atoms on carbon nanotubes (CNT) catalyst (Co-N 5 /CNT) was successfully fabricated via a low-temperature solvothermal reaction. The obtained Co-N 5 /CNT catalyst exhibited superior catalytic performance for PMS activation for sulfamerazine degradation. Its apparent rate constant k obs was 1.6 times higher than that of the Co-N 4 /CNT catalyst with four-coordinated nitrogen atoms prepared by the same method. Electron transfer non-radical mechanism was the main pathway for Co-N 5 /CNT to activate PMS. Higher single-atom cobalt metal loading (1.39 wt% vs 1.08 wt% in Co-N 4 /CNT) and significantly enhanced electron transfer ability (0.82 e vs 0.77 e in Co-N 4 /CNT) were the key factors for its superior catalytic performance. This work demonstrates a novel carbon-based single-atom cobalt catalyst for the removal of novel antibiotic contaminants by activating PMS in environmental catalysis applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Sijing Chen,Zhen Li,Longsheng Wu,Lu Liu,Jingping Hu,Huijie Hou,Sha Liang,Jiakuan Yang
Hemin has attracted considerable interest as an efficient catalyst recently, however, its direct application is inefficient due to severe molecular aggregation. Immobilizing hemin on various supports is a feasible approach to address this issue. In this work, a CNTs-hemin catalyst was prepared by loading hemin onto multiwalled carbon nanotubes (CNTs) through ball milling. Compared with hemin, CNTs-hemin demonstrates remarkably enhanced performance in the peroxymonosulfate system, with a 650-fold improvement of apparent rate constant, reaching 97.8% degradation of sulfathiazole in 5 min. High-valent iron-oxo porphyrin cation ((Porp) +• Fe IV =O) radicals are proposed as the dominant reactive species in the CNTs-hemin/peroxymonosulfate system instead of sulfate radicals (SO 4 •- ), hydroxyl radicals (•OH), superoxide radicals (O 2 •- ) and singlet oxygen ( 1 O 2 ). More in-depth mechanisms reveal that the strong electron transfer between CNTs and hemin promotes the generation of (Porp) +• Fe IV =O radicals through a heterolysis pathway. This research enriches the understanding of the catalytic mechanism of supported biomimetic catalysts for PMS activation and provides a perspective on the role of support materials for catalytic activity .
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MOLECULES
·
2023
·Vol. 28
·期 4
·1541
·
IF 4.6
Pascaline Sanga,Juanjuan Wang,Xin Li,Jia Chen,Hongdeng Qiu
Developing a simple and efficient method for removing organic micropollutants from aqueous systems is crucial. The present study describes the preparation and application, for the first time, of novel MXene-decorated bismuth ferrite nanocomposites (BiFeO3/MXene) for the removal of six sulfonamides including sulfadiazine (SDZ), sulfathiazole (STZ), sulfamerazine (SMZ), sulfamethazine (SMTZ), sulfamethoxazole (SMXZ) and sulfisoxazole (SXZ). The properties of BiFeO3/MXene are enhanced by the presence of BiFeO3nanoparticles, which provide a large surface area to facilitate the removal of sulfonamides. More importantly, BiFeO3/MXene composites demonstrated remarkable sulfonamide adsorption capabilities compared to pristine MXene, which is due to the synergistic effect between BiFeO3and MXene. The kinetics and isotherm models of sulfonamide adsorption on BiFeO3/MXene are consistent with a pseudo-second-order kinetics and Langmuir model. BiFeO3/MXene had appreciable reusability after five adsorption–desorption cycles. Furthermore, BiFeO3/MXene is stable and retains its original properties upon desorption. The present work provides an effective method for eliminating sulfonamides from water by exploiting the excellent texture properties of BiFeO3/MXene.Keywords:MXene;bismuth ferrite;nanocomposite;sulfonamide;adsorption
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ENVIRONMENTAL POLLUTION
·
2023
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IF 8.9
Rongqing Chen,Yunjia Liu,Jinlan Weng,Hua Huang,Xiaoying Gao,Zhipeng Wang,Jian Liu
The alteration of agricultural wastes into novel adsorbents can stimulate their scalability in realistic application, showing great economic and environmental advantages. Here, we proposed a strategy to engineer rice husk (RH) with microporous melamine-formaldehyde networks (MFNs) resins and the utilization for dynamic removal of organic micropollutants rapidly and efficiently. was pre-treated to acquire attractive surface and unique hierarchical porosity, endowing with surface functionalization and essential filtering properties. MFNs can be uniformly generated in-situ on the fully exposed cellulose backbones of the pre-treated RH. MFNs granules functionalized RH (RH@MFNs) exhibited high removal efficiencies over 90% within 30 min for the adsorption of hazardous organic compounds ( e.g., phenolic and antibiotic micropollutants) in static tests. Experiment results and density functional theory (DFT) simulation revealed that the synergy of hydrogen bonding, π-πinteraction, and micropore preservation dominates the adsorption. Further dynamic adsorption experiments showed that the removal efficiency and equilibrium removal capacity towards bisphenol A by RH@MFNs packed bed up-flow column were 2.6 and 67 times higher than that of raw RH, respectively. The column adsorption fits well with the Thomas model and bed depth service time (BDST) kinetic model. The inherent macropores inside RH and the roughness caused by the spiky structures and mesopores outside RH, as well as the accumulated MFNs granules, can lead to local turbulence of water flow around RH@MFNs, enabling fast and efficient adsorption. This sustainable and cost-effective preparation of RH-based adsorbents sheds light on the rational design of biomass waste adsorbents for realistic wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xuqian Wang,Linli Dai,Siyu He,Yabo Wang,Yongkui Zhang
Iron-based heterogeneous catalysts exhibit great peroxymonosulfate (PMS) activation ability to degrade persistent antibiotic pollutants, but the catalytic efficiency of this process is significantly affected by Fe(III)/Fe(II) conversion rate. Herein, we designed a novel biomineralization regulation process to fabricate graphene oxide modified schwertmannite composites (Sch-GO x ) as light-assisted PMS activator for enhancing sulfathiazole (STZ) degradation. More specifically, the introduction of GO in biomineralization process not only facilitated the dispersion of Sch, but also accelerated the regeneration of available surface-bound Fe(II) in resultant Sch-GO x through intramolecular electron transfer, thus promoting the activation of PMS. Compared with biosynthesized Sch without modification, the prepared Sch-GO 100 sample exhibited superior catalytic activity in light-assisted PMS activation process, 99.90 % removal efficiency of 78 μM STZ has been achieved within 30 min without pH adjustment (initial pH = 7.20). Abundant reactive oxygen species including SO 4 − , OH, O 2 − and 1 O 2 were responsible for the effective elimination of STZ. The potential degradation intermediates of STZ were investigated by liquid chromatography-mass spectrometry (LC-MS) and demonstrated to be less toxic than STZ using the ecological structure activity relationship program (ECOSAR). This study provided a facile and environmental-benign strategy of biomineralization regulation to fabricate effective iron-based PMS activator for environmental remediation.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Lixiang Zuo,Ran He,Li Wang,Yanli Wei
The fast and accurate detection of residual veterinary antibiotics in food has great significance for the ecological balance and human health. This study presents a room temperature phosphorescence aptasensing system for sulfadimethoxine (SDM) detection with sulfadimethoxine-aptamer (SDM-APT) modified manganese doped ZnS quantum dots (Mn-ZnS QDs) as the signaling and recognition unit. The signal amplification was achieved by petal-like molybdenum disulfide nano sheets (MoS 2 NS). As the selective adsorption of single-stranded DNA (ssDNA) on MoS 2 NS, SDM-APT-Mn-ZnS QDs are assembled on the surface of MoS 2 NS, and lead to the efficient phosphorescence quenching of Mn-ZnS QDs. Once SDM is brought in the sensing system, the specific interaction between SDM-APT and SDM will switch the conformation of SDM-APT from random coil to hairpin structure, resulting in the exfoliation of SDM-APT-Mn-ZnS QDs from MoS 2 NS, along with the phosphorescence recovery. This SDM detection system has a linear range from 2.0 ng/mL to 400 ng/mL with LOD as 0.91 ng/mL (S/N = 3) at the optimal experimental condition. The feasibility, specificity and recovery have been verified from the detection of real samples, interfering experiments and standard recovery experiments. The SDM detection system may also be applied to other residual veterinary drugs with different aptamers.
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Materials Today Communications
·
2022
·
IF 3.662
Shixing He,Lieshan Wu,Yalin Zeng,Bing Jia,Liuling Liang
Modified biochar (Ce-Ag-BC) was successfully prepared by using Camellia oleifera shell and doping with cerium (Ce) and silver (Ag). Through the results of BET, SEM, XRD , FTIR, and XPS, Ce and Ag were successfully embedded on biochar and participated in the sulfathiazole (STZ) adsorption. After being modified, high adsorption capacity of STZ on Ce-Ag-BC was observed. The maximum adsorption amount of STZ on Ce-Ag-BC was 261.84 mg/g, which was increased by more than six times compared to raw biochar (BC, 42.41 mg/g). The adsorption kinetics and isotherm on Ce-Ag-BC could be better fitted to pseudo-second-order kinetic and Langmuir isotherm model, respectively, indicating that the adsorption is mainly controlled by chemisorption and can be described as a monolayer process. The STZ adsorption process on Ce-Ag-BC is a spontaneously endothermic reaction. Besides, the adsorption mechanism on Ce-Ag-BC mainly involves pore filling, π-π interaction, hydrogen bonding , and electrostatic attraction.
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