MICROCHIMICA ACTA
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2020
·Vol. 187
·期 2
·1-8
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IF 6.232
Chen Lili,Xu Hui,Wang Li,Li Yong,Tian Xike
A novel ratiometric fluorescent probe for the determination of oxytetracycline (OTC) was developed. The method is based on the use of adenosine monophosphate/Eu(III) nanoscale coordination polymers doped with carbon dots (CDs) (CD@AMP/Eu NCPs). These were fabricated by self-assembly of Eu 3+ and AMP on the surface of CDs containing large amounts of hydroxyl and carbonyl groups. Under the excitation at 310 nm wavelength, the doped NCPs display strong pink emission of Eu 3+ at 615 nm and blue emission of the CDs at 430 nm on exposure to OTC. The ratio of fluorescence intensity (F 615 /F 430 ) of such NCPs displays excellent linear relationship with OTC concentration ranging from 0.2 to 60 μM and the limit of detection (LOD) is 25 nM (3σ). The doped NCPs were evenly immobilized on common filter paper to prepare a visual ratiometric probe for the determination of OTC. Assisted by a digital camera with an APP color detector, the paper-based test strip was applied for the quantitative determination of OTC with a LOD of 0.5 μM and a wide linear scope of 1–100 μM. The method was applied to the determination of OTC in milk samples.
Schematic representation of the principle for oxytetracycline (OTC) determination using carbon dots (CD)@adenosine monophosphate (AMP)/Europium (Eu 3+ ) paper-based ratiometic probe.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
Jianke Tang,Rongqian Meng,Yanfeng Xue,Shengjian Zhang,Qiaoling Li
A novel Ag 3 PO 4 /WO 3 ·H 2 O composite was prepared by loading Ag 3 PO 4 on WO 3 ·H 2 O substrate via a two-step hydrothermal method and characterized by various analytical techniques. The photocatalytic performance was evaluated by the degradation of methylene blue (MB) and oxytetracycline (OTC) under visible light irradiation. Within 30 min, 98.9 % MB can be degraded by the Ag 3 PO 4 /WO 3 ·H 2 O composite with a molar ratio of 3:1 (3Ag/1W), which is higher than that of individual Ag 3 PO 4 and WO 3 ·H 2 O. The 3Ag/1W photocatalyst also exhibits improved photocatalytic activity for OTC degradation than pure WO 3 ·H 2 O and Ag 3 PO 4 . The improvement of photocatalytic activity would be mainly ascribed to the highly efficient separation of photo-induced electron-hole pairs due to matched band structure, as confirmed by photoluminescence spectra (PL) and photocurrent responses test. According to the experimental results of radical trapping and electron spin resonance (ESR), a possible photocatalytic mechanism of the Ag 3 PO 4 /WO 3 ·H 2 O composite was proposed.
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MOLECULES
·
2024
·Vol. 29
·期 3
·659
·
IF 4.2
Zedian Li,Liangrui Xiang,Shijia Pan,Dahai Zhu,Shen Li,He Guo
This research constructed a novel O3/CaO2/HCO3−system to degrade antibiotic oxytetracycline (OTC) in water. The results indicated that CaO2andHCO3−addition could promote OTC degradation in an O3system. There is an optimal dosage of CaO2(0.05 g/L) andHCO3−(2.25 mmol/L) that promotes OTC degradation. After 30 min of treatment, approximately 91.5% of the OTC molecules were eliminated in the O3/CaO2/HCO3−system. A higher O3concentration, alkaline condition, and lower OTC concentration were conducive to OTC decomposition. Active substances including ·OH,1O2,·O2−, and ·HCO3−play certain roles in OTC degradation. The production of ·OH followed the order: O3/CaO2/HCO3−> O3/CaO2> O3. Compared to the sole O3system, TOC and COD were easier to remove in the O3/CaO2/HCO3−system. Based on DFT and LC-MS, active species dominant in the degradation pathways of OTC were proposed. Then, an evaluation of the toxic changes in intermediates during OTC degradation was carried out. The feasibility of O3/CaO2/HCO3−for the treatment of other substances, such as bisphenol A, tetracycline, and actual wastewater, was investigated. Finally, the energy efficiency of the O3/CaO2/HCO3−system was calculated and compared with other mainstream processes of OTC degradation. The O3/CaO2/HCO3−system may be considered as an efficient and economical approach for antibiotic destruction.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Rui Cheng,Shaowei Hu,Xiaochen Xu,Fenglin Yang
The algal-bacterial granular sludge (ABGS) system is an emerging wastewater treatment technology. With widespread coexistence of nanomaterials and antibiotics in the environment, their combined impact on wastewater treatment has attracted significant attention. In this study, oxytetracycline (OTC), ZnO nanoparticles (ZnO-NPs) and polystyrene nanoparticles (PS-NPs) were selected as model pollutants. The performance, microbial community, and variation in antibiotic resistance genes (ARGs) and mobile genetic elements (MGEs) of ABGS systems were explored under three long-term exposure (0.5 mg/L OTC, 0.5 mg/L OTC and 1 mg/L ZnO-NPs, 0.5 mg/L OTC and 1 mg/L PS-NPs). The results revealed that the coexistence of PS-NPs and OTC inhibited denitrification and phosphorus removal. ZnO-NPs addition promoted phosphorus removal efficiency (89.57 %±5.42 %), attributed to the hormesis of microalgae, low abundance of Competibacteraceae (0.2 %), and precipitation. The coexistence of nanomaterials and OTC increased reactive oxygen species and lactate dehydrogenase levels by 34.08–50.55 % and 3.56–60.82 % compared to that of single OTC stress (248.09 and 7.36 U/g·MLSS), indicating that nanomaterials enhanced OTC toxicity by disrupting cell membranes. The extracellular polymeric substance and adenosine triphosphatase overproduction of ABGS served as the defensive response to combined stress. The presence of nanomaterials, particularly PS-NPs, facilitated ARGs spread and proliferation, through significant MGE amplification (2.01 times) and increased abundance of potential hosts. This study underscores the importance of considering the role of nanomaterials in developing strategies to mitigate the ARGs spread and provides valuable insights into the effects of nanomaterial-antibiotic coexistence on ABGS systems.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Menglu Wang,Bolong Liang,Shumin Lin,Zhe Zhao,Hongbin He,Xiliang Li,Shu-xuan Liang
The magnetic Fe 3 O 4 @ZIF-8 with high adsorption properties and easy separation were embedded in BiOX (X = Cl, Br, I) to synthesize Fe 3 O 4 @ZIF-8@BiOX using a simple one-pot solvothermal strategy. The crystal structure, surface morphology, photoelectric properties, thermal stability and magnetic response of the three materials were compared and analyzed, and the effect on the removal of OTC and Cr(VI) from single and coexisting systems by adsorption-photocatalysis is discussed. The results show Fe 3 O 4 @ZIF-8@BiOI has the highest separation efficiency of photogenerated carriers upon photoexcitation and stronger light absorption capacity, and exhibits better adsorption-photocatalytic activity than the other two materials in the photocatalytic reduction of Cr(VI) (68 % and 65 % removal for single and coexisting systems) and degradation of OTC (86 % and 59 % removal for single and coexisting systems). It is noteworthy that in the coexistence of Cr(VI) and OTC, a slight decrease of removal occurred, which could be due to a competitive effect between two pollutants being greater than the synergistic effect. ∙O 2 - is the main active substances in the adsorption-photocatalysis process. Finally, this work demonstrates the excellent adsorption and photocatalytic ability of Fe 3 O 4 @ZIF-8@BiOI for the simultaneous removal of Cr(VI) and OTC, which has great potential for practical wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Su Xu,YaNi Yi,HuaYing Li,WeiWei Zhang
Oxytetracycline (OTC), a persistent and poorly biodegradable antibiotic, is increasingly detected in aquatic environments, posing ecological and health risks. Herein, a defect-rich, Co-free MoS₂/PMS system enables ultrafast OTC removal, achieving >99% elimination within 5 min (k obs = 0.791 min⁻¹). The process remained highly efficient across pH 2–10 and in real waters containing natural organic matter and common inorganic ions, demonstrating strong robustness under complex water matrices. Radical-quenching and electron paramagnetic resonance (EPR) analyses confirmed that •OH was the dominant reactive oxygen species (ROS), accompanied by SO₄•⁻ and ¹O₂. X-ray photoelectron spectroscopy (XPS) evidenced Mo⁴⁺/Mo⁶⁺ redox cycling and the participation of surface sulfur species and lattice oxygen, which jointly facilitated PMS activation and ROS generation, thereby establishing a coupled radical-non-radical degradation mechanism. Liquid chromatography–mass spectrometry (LC–MS) identified sequential demethylation, deamination, and ring-opening intermediates, while QSAR-based ecotoxicity assessment indicated an overall decrease in predicted toxicity for most transformation products relative to OTC. Machine-learning analysis (XGBoost with SHAP interpretation) highlighted reaction time, PMS dose, and natural organic matter as the primary determinants of degradation efficiency. Overall, this work integrates a Co-free, light-independent MoS₂/PMS system, refined dual radical–non-radical mechanistic elucidation, comprehensive toxicity mitigation assessment and explainable machine learning, offering both mechanistic and engineering guidance for the sustainable treatment of antibiotic-contaminated wastewater.
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Tong Wang,Xinyuan Wang,Xiao Wei,Mengwei Yan,Sihang Gao,Wenjuan Yang
Efficient sequestration of oxytetracycline (OTC) from aqueous environments is limited by the single interaction force of conventional adsorbents, stemming fundamentally from the insufficient understanding and translation of adsorption mechanisms into rational material design. In this study, based on the molecular structure complexity of OTC, a new type of waste-derived macroscopic adsorbent with high adsorption capacity was developed from the perspective of multi-site and multiple intermolecular forces synergy design. A covalent organic frameworks (COFs) rich in secondary amine, ketone, and sulfonic acid groups was grown in situ on peony pod-based cellulose-sodium alginate composite aerogel (PCSA). The composite PCSA@COFs showed an effective OTC adsorption capacity of 43.44 mg/g at 298 K, following pseudo-second-order and Langmuir models, indicating spontaneous, endothermic chemisorption. Density functional theory calculations further revealed a strong binding energy of −55.11 kcal/mol between COFs and OTC with multiple interaction sites. Topological analysis via Atoms in Molecules theory demonstrated a multi-site three-dimensional synergistic mechanism through the identification of ring critical points and cage critical points, while the topological parameters revealed a partially covalent character in the interaction between sulfonic acid groups and OTC. This work provides a novel design concept for developing effective and eco-friendly adsorbents for antibiotic removal from aqueous environments.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xin Qi,Zhuo Chen,Xiaotong He,Jiu-Qiang Xiong
The global challenge of antibiotic contamination calls for a comprehensive approach that integrates various technological, economic, and social factors to design effective, and sustainable solutions. Microalgae-based biotechnologies offer a sustainable and efficient approach to mitigating residual antibiotics while curbing the spread of antibiotic resistance genes. In this study, we found that the widely distributed microalgal species Chlamydomonas reinhardtii can efficiently degrade tetracycline, oxytetracycline (OTC), and doxycycline. Despite this promising result, the enzymatic mechanisms underlying this degradation process remain largely unknown. Taking OTC as a model chemical, we demonstrated that neither cytochrome P450 enzymes nor primary amine oxidase in C. reinhardtii were essential for OTC degradation using enzyme inhibition assays. Further identification and characterization of a novel tropinone reductase I (TRI) demonstrated that this enzyme catalyzes the demethylation of OTC, achieving a remarkable removal efficiency of 93.10% within 24 h. Additionally, informative analysis of metagenomic and metatranscriptomic databases revealed a widespread distribution and transcriptional activity of genes encoding TRI homologs across diverse environmental settings. The widespread distribution and transcriptional activity of TRI homologs suggest potential for TRI-mediated OTC degradation in diverse marine settings. These fundamental understandings of enzymatic catalysis processes not only provide critical insights into improving environmental management strategies, but also offer new lights on the unknown global impacts of novel phytoplankton enzymes.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shujuan Lian,Xiaoshuang Shi,Mingyi Lu,Mengdan Zhang,Xiaohuan Dong,Xu Li,Quan Feng,Rongbo Guo
Due to the persistence in residue and the emission to environment, antibiotics have become the emerging contaminants. Tetracyclines, as the largest amount of antibiotics in the breeding industry, were investigated in this study. For eliminating the tetracyclines, anaerobic culture was enriched from livestock waste after four generations and FeOn(OH)m modified oyster shell powders (OSPs) were amended into the enrichment culture as auxiliary method. Tetracycline and oxytetracycline were selected as the model compounds. The adsorption models (Langmuir and Freundlich isotherms) of tetracycline and microbes on OSPs were simulated respectively. With the addition of FeOn(OH)m modified OSPs, the transformation efficiency of oxytetracycline achieved 81.5% after 22 days’ incubation, approximately 1.85 times higher than the 4th generation (G-IV) enrichment culture without modified OSPs. Dehydration, demethylation, dehydroxylation and decarboxylation took place under anaerobic condition, inferred from the detected metabolites transformed from oxytetracycline. Genus Methanosarcina and two operational taxonomic units (OTUs) assigned to order Clostridiales , showed an increasing trend on abundance, indicating the contribution to transformation of oxytetracycline. Therefore, the FeOn(OH)m modified OSPs and enrichment culture can accelerate the transformation of oxytetracycline simultaneously, indicating a promising utilization not only for waste water system but also for antibiotic contaminated biomass treatment.
研究领域:
环境微生物学
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污染物生物降解
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环境工程
·
抗生素去除
·
吸附材料
·
厌氧消化
·
药物代谢
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Water
·
2022
·Vol. 14
·期 17
·2734
·
IF 3.53
Yuelin Xin,Peng Zhang,Jian Shen,Shaojie Ren
Oxytetracycline-containing wastewater, particularly produced by pharmaceutical industries, is too acidic to treat with iron-assisted materials. In order to tackle this issue, vitamin B6-mediated biochar with nano zero-valent iron coating (nZVI/B6@BC) was developed. Oxytetracycline (OTC) removal performance of biochar (BC), vitamin B6-coated biochar (B6@BC), nZVI-coated biochar (nZVI@BC), and vitamin B6-mediated biochar with nano zero-valent iron coating (nZVI/B6@BC) were investigated to analyze contributions and mechanisms of adsorption and degradation. Through modification, the adsorption capacity of B6@BC was slightly increased from 81.38 mg/g of BC to 85.64 mg/g. In the removal test, the 5-min OTC removal efficiencies with nZVI@BC and nZVI/B6@BC were 52.25% and 59.05%, yet the BC and B6@BC were limited to 5.61% and 8.54%. The distinct difference may be attributed to the existence of nZVI on biochar strongly improving the reactivity from adsorption to chemical reaction. Moreover, 98.28% of OTC was removed within 60 min in the nZVI/B6@BC suspension. The adsorption of OTC on BC fitted the Freundlich isotherm, Temkin isotherm, and intramolecular diffusion model, whereas that on B6@BC fitted Langmuir isotherm and pseudo-second-order better. Based on HPLC-MS analyses, there were three pathways proposed for OTC degradation in nZVI/B6@BC suspension. nZVI provided active sites on biochar for OTC degradation through oxidization, de-hydroxylation, ring-opening, reduction, addition, demethylation, and alkylation reactions. B6 as a mediate helped improve the stabilization and distribution of nZVI on biochar, which facilitates the capability of nZVI/B6@BC for OTC removal through adsorption and degradation under acidic conditions. The OTC can not only be captured on biochar but also be metabolized to achieve complete removal from aquatic systems.Keywords:oxytetracycline;biochar;nZVI;adsorption;degradation;acidic condition
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xuelian Hu,Ying Guo,Jinni Zhang,Xiaohui Wang,Guozhen Fang,Shuo Wang
Exploring high-performance fluorescence strategies for onsite monitoring of oxytetracycline (OTC) is of great significance for protecting human health. Herein, an innovative ratiometric fluorescence biomimetic sensor featured with high sensitivity and selectivity was constructed based on magnesium and nitrogen co-doped carbon dots embedded europium metal–organic framework and incorporating molecularly imprinted polymer (Mg,N-CDs/Eu-MOFs@MIP). In this protocol, MIP layer functioning as recognition units endowed Mg,N-CDs/Eu-MOFs@MIP with satisfactory binding efficiency and anti-interference ability. Mg,N-CDs/Eu-MOFs as both supporter and signal tag enabled the sensor to not only demonstrate a fast fluorescence response, but also yield reverse response signals depending on the synergistic effect of inner filter effect (IFE) and antenna effect (AE), achieving signal amplification. Benefiting from the efficient dual-channel strategy, Mg,N-CDs/Eu-MOFs@MIP exhibited a wide linear range (0.02–50 μg mL −1 ) with a sensitive detection limit (6.6 ng mL −1 ) and a marked color transformation (blue-to-red), which was highly desirable for monitoring of oxytetracycline. Simultaneously, aiming at attaining precise onsite analysis, a portable intelligent sensing platform was devised by integrating Mg,N-CDs/Eu-MOFs@MIP and a smartphone-assisted device. The smartphone with an installed color recognizer application as signal reader and analyzer realized oxytetracycline visual sensing by capturing and digitizing fluorescence images. More significantly, the portable platform was successfully applied to the onsite monitoring of OTC in water samples and milk samples with acceptable results. Accordingly, the as-developed platform demonstrated low-cost, portability, easy implementation, desirable specificity and sensitivity, presenting great potential for point-of-care testing.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2022
·
IF 8.91
Chengze Yu,Jiaqi Hou,Bin Zhang,Shiqi Liu,Xiangrui Pan,Heng Song,Xiangting Hou,Qinghua Yan,Chengzhi Zhou,Guocheng Liu,Yingjie Zhang,Yanjun Xin
The dual-chamber photoelectrocatalytic (PEC) system possess advantages in the degradation efficiency and processing cost of organic contaminants . In this study, TiO 2 nanotube arrays modified by rGO and g-C 3 N 4 (rGO/g-C 3 N 4 /TNAs) photoelectrodes were successfully prepared. The surface micromorphology , chemical structure, crystal structure, and basic element composition of rGO/g-C 3 N 4 /TNAs photoelectrodes were studied by SEM , FTIR, XRD , Raman, and XPS . UV–vis absorption, photoluminescence (PL) spectra, and photoelectrochemical (PECH) tests were used to explore the photoelectrochemical characteristics of rGO/g-C 3 N 4 /TNAs photoelectrodes. Under simulated sunlight illumination, the dual-chamber PEC system with external bias voltage was used to investigate the degradation of oxytetracycline (OTC) on rGO/g-C 3 N 4 /TNAs photoelectrodes. The results showed that rGO and g-C 3 N 4 were successfully loaded on TNAs, and the separation efficiency of electrons and holes at rGO/g-C 3 N 4 /TNAs photoelectrodes was improved. The light absorption range of rGO/g-C 3 N 4 /TNAs photoelectrodes extends to the visible light region and has better light absorption performance. Compared with the photocatalytic process, when 1.2 V bias voltage was applied, the degradation efficiency of OTC in anode and cathode chambers in PEC were increased by 3.28% and 44.01% within 60 min, respectively. In addition, the anode and cathode chambers have different degradation effects on OTC. Both the external bias voltage and initial pH have significant effects in cathode chamber, but have little effect in photoanode chamber. The fluorescence excitation-emission matrix spectra and liquid chromatography-tandem mass spectrometry showed that there were different intermediates in the degradation process of OTC. This study indicated that for the dual-chamber PEC system, rGO/g-C 3 N 4 /TNAs photoelectrodes exhibited excellent photocatalytic performance and have potential application prospects in water environmental remediation.
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