SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Huifang Wu,Yubing Chen,Mengqi Xu,Yuwei Ling,Shiying Ju,Yanfeng Tang,Changlun Tong
Tetracyclines residues, particularly oxytetracycline (OTC) and tetracycline (TC), have raised extensive concern because of their serious adverse effects on human health. Herein, a dual-response fluorescent probe based on nitrogen-doped carbon dots (N-CDs) and Eu 3+ hybrid (N-CDs–Eu 3+ ) was developed to selectively determine OTC and TC. The N-CDs act as ancillary ligands of Eu 3+ and recognition units of OTC/TC, while the Eu 3+ ions chelated with N-CDs can also specifically recognize OTC/TC. Upon inclusion of OTC/TC, an enhancement in Eu 3+ emission occurs due to the energy transfer from OTC/TC to Eu 3+ and the efficient elimination of quenching effect caused by H 2 O molecule, which is attributed to the incorporation of N-CDs; while the blue fluorescence emitted by the N-CDs decreases under the inner filter effect and static quenching effect caused by OTC/TC. Based on the double and reverse response signals, the ratiometric detection of OTC and TC in the range of 0.1–45 μΜ and 0.1–30 μΜ is achieved with a detection limit of 0.017 and 0.041 μM, respectively. In addition, the noticeable variation in fluorescence color of the probe is integrated with a smartphone-assisted analysis device for the rapid on-site quantitative assay of OTC, where the detection limit is 0.15 μΜ. The results show that this probe performs with excellent specificity and anti-interference for both OTC and TC, and satisfactory detection results are obtained in lake water, milk, and honey samples, thereby confirming that the probe exhibits promising application in food safety and environmental monitoring.
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PubMed
高影响因子
Materials Today Communications
·
2022
·
IF 3.662
Junyue Shan,Xianliang Wu,Caifang Li,Jiwei Hu,Zhenming Zhang,Huijuan Liu,Pinhua Xia,Xianfei Huang
In recent years, semiconductor materials have shown excellent potential in the field of photocatalytic degradation of antibiotics. To prepare a photocatalyst with excellent performance, an Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 tetrameric hybrid photocatalyst was successfully prepared for the first time by means of chemical precipitation using graphene oxide as the precursor. The developed quaternary photocatalyst was used for the degradation of oxytetracycline hydrochloride (OTC), and its photocatalytic activity was investigated. The structure and morphology of the composites were characterized by XRD , SEM, HR-TEM, ESR, N 2 adsorption, PL spectroscopy and UV-Vis DRS . The effects of different parameters on the degradation process were studied by the response surface method and artificial intelligence. The results showed that Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 was successfully synthesized. Under optimal conditions, the degradation rate of OTC was approximately 82% (the Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 dose was 0.16 g, the pH was 7.0, the initial concentration of OTC was 30 mg/L, and the visible light irradiation time was 70 min). pH is the most influential variable for OTC removal. At the same time, the degradation rate of OTC remained above 50% after 5 times of recycling, indicating that Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 photocatalyst had good stability and recoverability. In addition, the results of ESR and radical trapping experiments showed that·O 2 - and·OH were the main active species in the OTC removal process.
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Environmental Science-Water Research & Technology
·
2022
·Vol. 8
·期 8
·1763-1776
·
IF 5.819
Di Li,Mingyang Long,Qianqian Zhao,Hongmiao Li,Qi Wen,Fang Song
Nanosized CoTiO3, NiTiO3 and Fe2TiO5 photocatalysts were synthesized by a simple sol–gel method successfully. However, they showed lower photocatalytic activity for the degradation of oxytetracycline hydrochloride under visible light irradiation. After the CoTiO3, NiTiO3 and Fe2TiO5 nanoparticles were loaded in the SBA-15 channels, the photocatalytic activity was enhanced obviously. In order to further enhance the removal efficiency of CoTiO3/SBA-15, NiTiO3/SBA-15 and Fe2TiO5/SBA-15, they were used to activate peroxymonosulfate under visible light irradiation. In particular, CoTiO3/SBA-15 could completely photodegrade oxytetracycline hydrochloride with the assistance of peroxymonosulfate in an hour. The influencing factors on activating peroxymonosulfate to degrade oxytetracycline hydrochloride were investigated in detail. In addition, the electron transfer and peroxymonosulfate activation mechanism for the efficient improvement in the photocatalytic performance were also proposed and proved by radical quenching experiments, electron spin resonance analysis, X-ray photoelectron spectroscopy, transient photocurrent responses and cyclic voltammetry. It was found that the combined activation effects of photogenerated electrons and transition metals on peroxymonosulfate to produce sulfate radicals could enhance the degradation efficiency obviously. This study could provide a new way for the synergetic effect of photocatalysis and peroxymonosulfate activation by transition metal to be used for efficient photocatalytic degradation in the field of antibiotic removal.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Dan Zhang,Shengke Yang,Chunyan Yang,Yangyang Chen,Ruixin Hu,Yali Xie,Yanhua Wang,Wenke Wang
Dissolved organic matter (DOM) is composed of numerous fluorescent components. It is an indispensable parameter to affect the environmental fate of antibiotics in various ways. To assess the migration of antibiotics in environment compartments, it is crucial to understand the binding mechanism between DOM and antibiotics. How a particular component in DOM interacts with coexistence antibiotics is not still fully understood. Therefore, in the present study, interactions of two antibiotics oxytetracycline (OTC) and sulfadiazine (SD) with humic acid (HA) and L-tryptophan (L-Trp) which were representative DOM components, were investigated by multispectral techniques and density functional theory (DFT) calculations. The fluorescence quenching mechanism was static quenching. In the binding process, the quenching ability of OTC was stronger than that of SD in HA, which was the same as in L-Trp. DFT calculations were applied to confirm a stronger interaction between OTC and HA or L-Trp than SD. Meanwhile, analyzing the binding sequence by two-dimensional correlation spectroscopy (2D-COS), a humic-like substance bound antibiotics was earlier than a protein-like substance. In HA system, the combination of two antibiotics had a synergistic effect on HA quenching. In L-Trp system, the quenching relationship between the two antibiotics and L-Trp was antagonistic. The FTIR spectra showed that hydroxyl and amide were involved in the binding process of individual DOM components with OTC and SD. The work will help to further understand the behavior of coexistence antibiotics in the environment.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yu Wang,Yuxin He,Yujing Chi,Peiji Yin,Lishan Wei,Wenwen Liu,Xinyao Wang,Han Zhang,Haiyan Song
Photocatalytic H 2 O 2 production is a green and sustainable technology, which still exposes the issues of excessive dependence on organic electron donors and pure O 2 , and lacking effective use. It is necessary to develop more efficient and more economical photocatalysis system for H 2 O 2 production. Here, we construct a S-scheme p-n heterojunction from the p-type MnS and the n-type protonated g-C 3 N 4 (PCN) semiconductors for photocatalytic H 2 O 2 production and achieve the in situ use of H 2 O 2 for oxidative degradation of oxytetracycline (OTC). The PCN/MnS composite synthesized by a one-step method well maintains a nanosphere structure of α-MnS and load the PCN on the sphere surface to form a heterojunction with strong interaction. PCN/MnS exhibits the improved photogenerated charge separation and electron transfer efficiency. An optimal photocatalyst can produce 669.6 μM of H 2 O 2 for 6 h without using the electron donors and the pure O 2 gas. The mechanism proposed the contribution of a S-scheme p-n heterojunction forms between PCN and MnS. The electrons in conduction band (CB) of MnS are responsible for the major single-electron reduction of •O 2 - radicals and the auxiliary two-electron reduction of O 2 for H 2 O 2 production, while the holes in valence band (VB) of PCN further promote the separation of photocarriers. The photogenerated H 2 O 2 can be effectively used as an in-situ oxidant to achieve 82.2% degradation of OTC in water within 80 min. The •O 2 - radicals which originate from the in situ decomposition of H 2 O 2 over PCN/MnS mainly contribute to the OTC oxidation .
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xiangdong Zhang,Jian Zhang,Bowen Hou,Xueying Yang,Junlian Ren,Chen Shao
Selective removal of organic pollutants by PMS-activated heterogeneous catalytic system has become one of the commonly used methods, but the adsorption of the catalyst is often ignored in the degradation process. Metal-organic frameworks (MOFs) are often used in the field of environment because of their high porosity and structural diversity/adjustability. However, there are still difficulties in the aggregation and recycling of nanoparticles . This study effectively synthesized the material CuS-PVP@ZIF-67 by using hollow spherical CuS as the carrier of Co-MOF (ZIF-67) to solve these problems. A high concentration of oxytetracycline hydrochloride (OTC) can be successfully adsorbed by electrostatic attraction and π-π interaction, and small amount of PMS may be quickly activated, and the removal rate of OTC is 94.82 % in 20 min. The catalyst used can be easily recovered by suction filtration and has good reusability. In addition, a potential cooperating mechanism for adsorption-PMS activation has additionally been proposed. The degradation pathway of OTC is determined, and the potential harm of intermediate products is analyzed. This work aims to create a heterogeneous catalytic system with significant adsorption and catalytic ability to remove refractory organic contaminants in water.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2021
·Vol. 96
·期 6
·1580-1592
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IF 3.174
Yicheng Dou,Xingyu Shen,Jinte Zou,Runzhe Shi,Tingting Yan,Qiya Sun,Lin Wang
BACKGROUND In this study, sulfur-doped g-C 3 N 4 (SCN) nanosheets were synthesized using thiourea as a precursor, and then used to catalyze the degradation of oxytetracycline (OTC) under visible-light irradiation. OTC was chosen as target contaminant because of it being an important precursor of N -nitrosodimethylamine (NDMA). RESULTS The removal of OTC was influenced by its initial concentration, initial pH, SCN dosage and water matrices. OTC (≤10 mg L −1 ) was almost completely removed in 40 min under the conditions of an initial pH of 7.0 and a SCN dose of 1.0 g L −1 , and its degradation was well described by the pseudo-first-order kinetics model. Water matrices would also influence the degradation of OTC in the system. Electron paramagnetic resonance analysis and trapping experiments confirmed that the function of the radicals for OTC removal followed the order of • O 2 − > • OH > h + . Eight transformation products were determined during the degradation of OTC, it being removed through four pathways: methyl oxidization, demethylation, decarbonylation and secondary alcohol oxidation. SCN was stable in the system, as the removal efficiency of OTC was not significantly reduced even after three recycles. In addition, 55.5% of NDMA formation potential of OTC was reduced after SCN catalytic oxidation. CONCLUSIONS The results imply that the visible-light-driven SCN catalytic oxidation is an effective technology not only for the removal of OTC but also for the reduction of NDMA formation potential. © 2021 Society of Chemical Industry
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Antibiotics-Basel
·
2020
·Vol. 9
·期 12
·874
·
IF 3.893
Chuanyu Yang,Hanqing Hu,Yihong Wu,Xiongjie Lin,Goucheng Fan,Yongping Duan,Charles Powell,Veronica Ancona,Muqing Zhang
Citrus huanglongbing (HLB) is a devastating disease for the citrus industry. The previous studies demonstrated that oxytetracycline and penicillin are effective antibiotics againstCandidatusLiberibacter asiaticus (CLas). However, sinceCLas is uncultured, the mechanisms of action of antibiotics againstCLas are still unclear. It was recently reported that the endophytic microbial communities are associated with the progression of citrus HLB after oxytetracycline and penicillin treatment. Therefore, we hypothesize that penicillin has greater antibacterial activity againstCLas than oxytetracycline, which may be associated with the alteration of the structure and function of endophytic microbial communities in HLB-affected citrus in response to these antibiotics. To test this hypothesis, the microbiome of HLB-affected citrus leaves treated with these two antibiotics was analyzed using a metagenomic method. Our results indicate that the microbial structure and function in HLB-affected citrus were altered by these two antibiotics. The relative abundance of beneficial bacterial species, includingStreptomyces avermitilisandBradyrhizobium,was higher in penicillin-treated plants compared to those treated with oxytetracycline, and the relative abundance of the bacterial species (such asPropionibacterium acnesandSynechocystissp PCC 6803) associated withCLas survival was lower for penicillin-treated plants compared to oxytetracycline-treated plants. These results indicate that penicillin has greater antibacterial activity againstCLas. Based on the metagenomic analysis, this study elucidated the mechanism for the observed increase in antibacterial activity of penicillin againstCLas. The data presented here are not only invaluable for developing eco-friendly and effective biocontrol strategies to combat citrus HLB, but also provide a method for revealing mechanism of antimicrobial against uncultured bacteria in host.Keywords:citrus Huanglongbing;endophytic microbiome;oxytetracyline;penicillin;mode of action
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Xiangyu Zhang,Tongyun Yin,Zhengquan Chen,Yunchuan Long,Juan Jiang,Shaoqi Zhou,Jing Hu,Shengming Ma
The activation mechanism and degradation mechanism of peroxydisulfate (PDS)-based advanced oxidation technologies in applications have received increasing attention. In this paper, N,B co-doped biochar graphene (N,B-rGO-900) was synthesised from discarded coconut shells, which showed good adsorption and catalytic properties in the removal of oxytetracycline (OTC), there is no energy barrier to impede the electron transfer process. The adsorptive removal rate was 53 % in 30 min, and the degradation rate was 94.14 % in 15 min, with a reaction rate constant of 0.1363 min −1 (k 0- 15min ), which was higher than the degradation rate(47 %) in 15 min for N-rGO with an energy barrier of 0.215 eV. More importantly, this study clarifies the structure–activity relationship of the catalyst, in the radical pathway, the number of electrons transferred to the PDS from the lone pairs of pyrrolic N and pyridinic N on N,B-rGO-900 was 0.045 e, which was higher than that of N-rGO (0.032 e) and pristine GO (0.019 e), contributing to the decomposition of PDS to produce radicals; in contrast, the N,B-rGO-900 in the nonradical pathway acts as an electron channel to promote electron migration from OTC to surface-confined N,B-rGO/PDS* complexes, the electron migration is driven by the potential energy difference between the highest occupied molecular orbital (HOMO, −4.932 eV) and the lowest vacant molecular orbital (LUMO, −1.923 eV), a process in which PDS extracts 2 electrons to the OTC, while ketones or quinones in the catalyst can act as Lewis acid sites to activate PDS to produce 1 O 2 , in addition the introduction of N and B atoms reduces its activation energy in the reaction process (Ea = 45.45 kJ mol −1 ). The highest contributing active substance in the degradation process was O 2 • − (97 %) in the free radical pathway, and it was capable of degrading OTC into small molecules that are non-toxic to fish, daphnid, and algae, toxic concentrations much greater than 100 mg/L, and the catalyst was able to maintain an excellent performance after four reuse experiments and anti-interference experiments. This study systematically elucidates the process mechanism of antibiotic degradation by persulfate and provides new insights into the design of economic, efficient and stable targeted carbonaceous catalysts.
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高影响因子
Sustainability
·
2021
·Vol. 13
·期 7
·4014
·
IF 3.251
Zijing Fan,Mei Zhang,Xiaxia Chen,Zhongda Hu,Qihang Shu,Chaosen Jing,Xingzhang Luo
Oxytetracycline (OTC) is a commonly used antibiotic in livestock farming for controlling intestinal and respiratory infections in farm animals. However, the absorption of antibiotics by animals is limited, and most antibiotics are excreted in the original form with manure, which will have an impact on the environment. The removal of antibiotics from swine manure could generally be performed via anaerobic digestion (AD). In this study, the effect of oxytetracycline (OTC) at doses of 0.1, 0.5, and 1.0 mg/L on the thermophilic anaerobic digestion of swine manure (55 °C) in batch digesters was studied. The methane production, volatile fatty acid (VFA) levels, and dissolved organic matter (DOM) were determined and compared with the control (0 mg/L of OTC). The results indicate that (1) OTC at 0.1 mg/L had no inhibitory effect on methane production or on the accumulation of VFAs, while 0.5 mg/L and 1.0 mg/L inhibited methane production, with inhibition rates of 4.03% and 14.12% (p< 0.05), respectively; (2) the VFAs of each reactor peaked on the first day of the reaction, and as the OTC dose increased from 0 to 1.0 mg/L, the maximum VFA accumulation increased from 1346.94 mg/g to 2370 mg/g of volatile solids (VS); and (3) oxytetracycline (0.5 and 1.0 mg/L) could promote the temporary accumulation of propionic acid, which did, however, not result in significant VFA accumulation. Further, OTC at 1.0 mg/L can promote DOM production, and therefore, VFA accumulation.Keywords:thermophilic anaerobic digestion;oxytetracycline;volatile fatty acids;methane production;swine manure
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高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2025
·
IF 4.7
Xinglin Li,Pengfei Zhu,Yu Chen,Maojie Zhang,Yunhui Jiang
In this paper, Co 2+ was successfully assembled into a complex by solvothermal method with meso-tetra (4-carboxyphenyl) porphyrin (TCPP), and then a novel P/BiOIO 3 /Co-TCPP inorganic-organic composite photocatalytic material was prepared by one-pot solvothermal method. It was found that after 60 min of reaction under visible light, the degradation rate of the preferred P/BiOIO 3 /Co-TCPP composite material for 20 mg/L oxytetracycline hydrochloride (OTC) reached 88.15 %, with its pseudo-first-order kinetic model fitting constant measured at 0.03852 min −1 . It was 5.12 and 1.52 times that of BiOIO 3 and P-doped BiOIO 3 respectively, and there was no significant decrease in activity after three consecutive uses. Meanwhile, the noxiousness of the OTC solution after photocatalytic degradation by this catalyst was significantly reduced. The characterization results indicate that the primary factor contributing to the improved activity is the P/BiOIO 3 /Co-TCPP catalyst can be attributed to the doping of BiOIO 3 by P and the coupling of Co-TCPP to BiOIO 3 , which significantly improves the catalyst's response ability to visible light. Meanwhile, P/BiOIO 3 and Co-TCPP form a Z -scheme heterojunction, which greatly facilitates the separation of photogenerated carriers. Finally, the electron transfer mechanism and possible degradation pathways of the photocatalytic degradation of OTC by P/BiOIO 3 /Co-TCPP were proposed. This study provides a feasible and effective method for the modification of BiOIO 3 -based heterojunction photocatalysts and the treatment of antibiotics in water bodies.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kamile Arkin,Yuxin Zheng,Yuyang Bei,Xuesong Ma,Weilong Che,Qingkun Shang
In this work, blue carbon dots (Stalk-Trp CDs) with high fluorescence quantum yield were successfully prepared from biological waste cherry tomato stalk and tryptophan. The morphology, composition, and properties of Stalk-Trp CDs were characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, infrared spectroscopy, ultraviolet–visible absorption spectroscopy, and fluorescence spectroscopy. On this basis, a dual-channel ratio sensing platform (Stalk-Trp CDs@Eu) was constructed using the interaction of Stalk-Trp CDs with Eu 3+ , which reduced the detection limit of the antibiotic oxytetracycline from 0.15 µmol/L to 0.018 µmol/L. Channel 1 of the dual-channel ratio sensing platform is a neutral environment (pH = 6.5), and the specific response of the probe to OTC causes its fluorescence to change from blue to purple. Channel 2 is an alkaline environment (pH = 11.5), and the fluorescence of the probe turns green only in the presence of OTC. The interaction mechanism of the dual-channel ratio sensing platform with the antibiotics oxytetracycline (OTC), chlortetracycline (CTC), and tetracycline (TC) was also revealed. The detection results of OTC in honey and milk by using Stalk-Trp CDs@Eu were highly consistent with the HPLC method recommended by the national standard. This shows that the dual-channel ratio sensing platform has great practical application value in the field of antibiotic detection.
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危险品化学品经营许可证（带存储）