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Royal Society Open Science · 2021 ·Vol. 8 ·期 8 · IF 2.963

Effective removal of tetracycline antibiotics from wastewater using practically applicable iron(III)-loaded cellulose nanofibres

Lanxin Lu,Min Liu,Ying Chen,Ying Luo

The non-toxic and completely biodegradable cellulose within bamboo is one of the most abundant agricultural polysaccharide wastes worldwide, and can be processed into cellulose nanofibres (CNFs). Iron(III)-loaded CNFs (Fe(III)@CNFs) derived from bamboo were prepared to improve the adsorption of tetracycline (TC), chlortetracycline (CTC) and oxytetracycline (OTC) from an aqueous solution. The preparation conditions of Fe(III)@CNFs suitable for the simultaneous adsorption of three tetracycline antibiotics (TCs) were investigated. Various analyses proved the abundance of oxygen-containing functional groups and the existence of Fe(III) active metal sites in Fe(III)@CNFs. In batch experiments, Fe(III)@CNFs were applied under a wide pH range and the maximum adsorption capacities were 294.12, 232.56 and 500.00 mg g−1 (for TC, CTC and OTC, respectively). In addition, different concentrations and types of coexisting anions have a weak effect on TCs adsorption. The original TCs adsorption capacities of Fe(III)@CNFs remained stable (greater than 92%) after five cycles when UV + H2O2 was used as the regeneration method. Four adsorption mechanisms (surface complexation, hydrogen bonding, electrostatic interaction and van der Waals force) were obtained for the endothermic adsorption of TCs, among which surface complexation between Fe(III) and TCs always dominates. The practically applicable Fe(III)@CNFs adsorbents are promising for TCs enrichment and remediation in engineering applications.

CAS / MDL: 2058-46-0 393781-70-9
研究领域: 环境科学 · 材料科学
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Water · 2021 ·Vol. 13 ·期 24 ·3497 · IF 3.103

The Effect of Exogenous Oxytetracycline on High-Temperature Anaerobic Digestion of Elements in Swine Wastewater

Zhongda Hu,Zijing Fan,Qixuan Song,Rabia Khatoon,Mei Zhang,Ning Wang,Xingzhang Luo

Tetracycline antibiotics (TCs) are a common type of antibiotic found in swine wastewater. Oxytetracycline (OTC) is a significant type of TC. This study mainly examined the influence of OTC on high-temperature anaerobic digestion by adding OTC to collections of swine wastewater at different times during the digestion process. The results showed that high-temperature anaerobic digestion was suitable for the removal of TCs, with an 87% OTC removal efficiency achieved by day 20. Additionally, OTC added from external sources was found to inhibit the chlortetracycline degradation process and affect the first-order degradation kinetic model of TCs. Complexation reactions were the main ways in which OTC affected the heavy metal content of the water. The exogenous addition of OTC was found to inhibit the activity of some digester microbial strains, reduce the proportion of dominant strains, such asMBA03, and kill certain specific strains. This performance alteration was most obvious when OTC was added in the middle of the reaction.Keywords:swine wastewater;high-temperature anaerobic digestion;tetracycline antibiotics;oxytetracycline

研究领域: 环境工程 · 微生物学
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RSC Advances · 2016 ·Vol. 6 ·期 113 ·112166-112174 · IF 3.289

Preparation of magnetic activated carbon from waste rice husk for the determination of tetracycline antibiotics in water samples

Jianqiu Lou,Xin Xu,Yunfang Gao,Dezhou Zheng,Jinyang Wang,Zuguang Li

In this work, the silica in rice husk was removed to create a natural template to prepare porous activated carbon. The preparation process of the activated carbon (AC) from waste rice husk consisted of carbonization, silica removal and activation. Factors affecting the preparation of AC, including the mass ratio of ZnCl2 and rice husk carbon (RHC), activation temperature and time were investigated. Based on the Brunauer–Emmett–Teller (BET) results, the specific surface area of AC prepared under optimized conditions was as high as 1673.25 m2 g−1. Then, magnetic activated carbon (mag-AC) was synthesized by in situ co-precipitation of rice husk-based activated carbon and Fe3O4. The specific surface area and average pore diameter of mag-AC were respectively 986.97 m2 g−1 and 3.62 nm, respectively. It was shown that mag-AC was a viable adsorbent for magnetic extraction of tetracycline antibiotics in water samples followed by quantification by HPLC-MS/MS. The results indicated satisfactory correlation coefficients (R2) ranging from 0.9955 to 0.9998. Limits of detection (LOD) and quantization (LOQ) were achieved in the range of 0.10 to 0.95 and 0.35 to 2.85 μg L−1 in water samples, respectively.

CAS / MDL: 10025-77-1 7758-94-3
研究领域: 环境科学 · 分析化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Oxygen Vacancy Formation Energy Determines the Phase-Activity Relationship of MnO2 Laccase Nanozymes

Qing Tian,Haoyu Wang,Shuaiqi Huangfu,Rong Yang,Yao Chen,Jie Gao,Yingchun Yang,Lianbing Zhang

Although manganese dioxide (MnO2) has been explored as a powerful laccase nanozyme for pollutant oxidation in wastewater treatment, the phase-activity relationship of multiphase MnO2 remains ambiguous and controversial. Herein, the experimental studies show that the laccase-like activities and aerobic catalytic oxidation toward tetracycline antibiotics of the six types of MnO2 are in the following order: β- > λ- > γ- > α- > ε- > δ-MnO2. Density functional theory (DFT) calculations revealed that the catalytic activities are inversely proportional to the oxygen vacancy formation energies of the different MnO2 materials. Further investigation of surface oxygen species with reactivity demonstrated that rich oxygen vacancies boost the oxygen mobility and catalytic efficiency of MnO2 nanozymes, which is in good agreement with both experimental and DFT results. Hence, this study reveals the decisive role of the crystal phase in the oxygen vacancy generation, which elucidates the laccase-like catalytic mechanism of MnO2 nanozymes and is valuable for the future design and synthesis of MnO2 nanocatalysts.

研究领域: 环境科学 · 材料科学 · 生物学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

Metal-mediated chitosan@mesoporous silica-based ultrasensitive fluorescent probe for the ratiometic and colorimetric detection of tetracycline antibiotics

Lina Gao,Junfei Wu,Hai-Bo Liu,Qian Zhao,Jing Wang

Naphthalimide-functionalized chitosan and mesoporous SBA-15 silica were integrated by forming CS–HNB@SBA nanocomposites. SBA-15 served as a solid matrix that enabled good water dispersibility and reusability. To achieve distinction between tetracycline (TET) and oxytetracycline (OTC), CS–HNB@SBA and rhodamine derivative-modified SBA-15 constructed a fluorescent ensemble. To improve determination accuracy and sensitivity, multiple recognition sites (Eu 3+ and Zn 2+ ) were incorporated to build metal-mediated sensing systems. When tetracycline antibiotics (TCs) were present, blue emission of naphthalimide at 389 nm was quenched based on Förster resonance energy transfer, whereas characteristic peak of Eu 3+ at 619 nm (or TCs Zn 2+ at 527 nm) was enhanced through antenna effect (or chelation of TCs and Zn 2+ ) based on “CS–HNB@SBA-metal ion-TCs” ternary complex. Fluorescent color displayed obvious changes from blue to red (or green), showing a huge potential for visual determination. Ultra-low detection limits of TET (or OTC) were 0.048 (or 0.064 nM) and 0.072 nM (or 0.042 nM), respectively, by using CS–HNB@SBA/Zn 2+ and CS–HNB@SBA/Eu 3+ , respectively, due to their amplified and synergistic fluorescence signals. This work enriches the strategy for constructing ultrasensitive fluorescent probes by taking advantage of cooperative effect of multiple recognition sites, and offers insights into efficient ensemble platforms for structurally similar analytes.

研究领域: 分析化学 · 环境科学 · 生物医学工程
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RSC Advances · 2016 ·Vol. 6 ·期 111 ·109983-109991 · IF 3.289

Equilibrium, isotherm, kinetic and thermodynamic studies for removal of tetracycline antibiotics by adsorption onto hazelnut shell derived activated carbons from aqueous media

Hong-Tao Fan,Li-Qi Shi,Hua Shen,Xi Chen,Kun-Peng Xie

Hazelnut shell, an agricultural waste, was used to prepare activated carbons by phosphoric acid activation. Hazelnut shell derived activated carbon (HSAC) was characterized by Fourier transform infrared spectroscopy, Raman spectroscopy, scanning electron microscopy and N2 adsorption/desorption isotherms, and was used as an adsorbent for the removal of three tetracycline (TC) antibiotics (tetracycline (TC), oxytetracycline (OTC), and chlortetracycline (CTC)) from aqueous solution. Batch adsorption studies were carried out by varying the initial concentrations of TCs, pH of solution, ionic strength of solution, contact time and temperature. 20 min was required to attain equilibrium. There was no significant influence of ionic strength in a range from 0.0001 to 1 mol L−1 and pH in the range of 4–8 on the uptakes of TCs by the HSAC. The maximum adsorption capacities of the HSAC followed the sequence OTC (321.5 mg g−1) > CTC (313.5 mg g−1) > TC (302.9 mg g−1). The data fitted well with the pseudo-second-order kinetic and Langmuir models. The intraparticle diffusion model indicated that the adsorption of TCs on the HSAC was controlled by both intraparticle diffusion and external mass transfer. Under the test temperature and pressure, the thermodynamic constants revealed that the adsorption of TCs onto the HSAC was spontaneous and endothermic. The HSAC had relatively high potential for the removal of TCs from aqueous solution.

研究领域: 环境科学 · 生物学
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JOURNAL OF MOLECULAR STRUCTURE · 2025 · IF 4.7

A novel fluorescent probe based on dicyanoisophorone for the detection of tetracycline antibiotics and its application to water samples

Linxiu Zhao,Yue Zhao,Yuqi Wu,Taisheng Zhu,Yuxin Miao,Tongtong Zhang,Shengling Li,Jianlan Cui

Antibiotics play an irreplaceable role in controlling bacterial infections and safeguarding human health. However, the misuse of antibiotics in animal husbandry and aquaculture has caused widespread ecological contamination. Specifically, tetracycline antibiotics (Tetracyclines, TCs), as one of the most prevalent antibiotic residues, pose significant risks to environmental sustainability and food safety. To address this issue, we developed a novel dicyanoisophorone-based fluorescent probe, ( E )-2-(3-(2-(5-formyl-6-hydroxy-2-naphthalenyl)vinyl)-5,5-dimethylcyclohex-2-en-1-yl)malononitrile ( ZHP ), enabling rapid and selective detection of TCs. Notably, ZHP exhibited distinct fluorescence responses toward different TCs: fluorescence quenching upon binding to chlortetracycline (CTE) (detection limit: 9.6 µM) and fluorescence enhancement in the presence of doxycycline (DOX), oxytetracycline (OXY), and tetracycline (TET) (detection limits: 0.23 µM, 0.24 µM, and 0.39 µM). This differential response mechanism, potentially attributed to structural variations among TCs. The probe demonstrated excellent pH tolerance (pH 6 - 12) and high selectivity over 6 common interfering antibiotics. A paper-based colorimetric assay achieved visual TCs detection within 5 seconds, highlighting its field-deployable potential. Furthermore, the probe ZHP was successfully applied to quantify TCs in different water samples with recoveries of 96.33 - 103.00%. This work provides a sensing platform for TCs monitoring, offering critical insights into the design of multifunctional probes for environmental applications.

CAS / MDL: 10026-22-9
研究领域: 环境科学 · 分析化学
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CHEMOSPHERE · 2021 · IF 7.086

Rice straw particles covered with Brevundimonas naejangsanensis DD1 cells can synergistically remove doxycycline from water using adsorption and biotransformation

Ting He,Jianguo Bao,Yifei Leng,Shuqiong Kong,Jiangkun Du,Xu Li

Doxycycline (DC) is a second generation tetracycline antibiotic and its occurrence in the aquatic environment due to the discharge of municipal and agricultural wastes has called for technologies to effectively remove DC from water. The objective of the study was to characterize the synergistic benefits of adsorption and biotransformation in removing DC from water using rice straw particles (RSPs) covered with DC degrading bacteria, Brevundimonas naejangsanensis strain DD1. First, optimal experimental conditions were identified for individual processes, i.e., hydrolysis, adsorption, and biotransformation, in terms of their performance of removing DC from water. Then, synergistic effects between adsorption and biotransformation were demonstrated by adding DD1-covered RSPs (DD1-RSPs) to DC-containing solution. Results suggest that DC was quickly adsorbed onto RSPs and the adsorbed DC was subsequently biotransformed by the DD1 cells on RSPs. The adsorption of DC to DD1-RSPs can be well described using the pseudo-second-order kinetics and the Langmuir isotherm. The DD1 cells on RSPs converted DC to several biotransformation products through a series of demethylation, dehydration, decarbonylation, and deamination. This study demonstrated that adsorption and biotransformation could work synergistically to remove DC from water.

CAS / MDL: 75-05-8 67-56-1
研究领域: 环境科学 · 微生物学
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MICROCHIMICA ACTA · 2024 ·Vol. 191 ·期 3 ·1-11 · IF 5.3

Fluorimetric determination of tetracycline antibiotics in animal derived foods using boron and nitrogen co-doped ceria-based nanoparticles

Li Qianji,Fan Pengfei,Hao Zejia,Ni Shanhong,Wu Qian,Li Lei

An innovative synthesis of boron and nitrogen co-doped ceria-based nanoparticles (B/N-CeFNPs) with bright blue fluorescence emission is reported using the hydrothermal method. Based on the aggregation-induced emission enhancement (AIEE) effect between B/N-CeFNPs and chlortetracycline (CTC), a rapid detection method for CTC through fluorescence enhancement was developed. In addition, through the electron transfer process (ET), fluorescence resonance energy transfer (FRET) effect and static quenching between B/N-CeFNPs and oxytetracycline (OTC), a ratio fluorescence strategy for detecting OTC was generated. The fluorescence of B/N-CeFNPs at 410 nm can be effectively quenched by OTC, and new fluorescence emission appears at a wavelength of 500 nm. B/N-CeFNPs showed good linear responses with CTC and OTC in the range 0.1-1 µM and 1-40 µM, respectively. This system was used to simultaneously detect the CTC and OTC in milk and honey, realizing multi-residues detection of TCs in actual samples by using the same ceria-based fluorescence nanomaterial. Graphical abstract

研究领域: 分析化学 · 食品科学
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INORGANIC CHEMISTRY COMMUNICATIONS · 2024 · IF 4.4

Room-temperature synthesis of Fe/Cu-BTC for effective removal of tetracycline antibiotic from aquatic environments

Wei Xiang,Yueting Liao,Jinwei Cui,Yangyang Fang,Bining Jiao,Xuesu Su

Antibiotic adsorbents are getting significant attention due to the hazards posed by the accumulation of tetracycline antibiotics in water, which can adversely impact human and environmental health. Bimetallic organic frameworks (BMOFs) exhibit considerable potential in adsorption owing to their dense pore structures and synergistic effects. However, synthesizing efficient, low-cost, and easy-to-prepare BMOFs faces several challenges. Here, we describe the practical synthesis of a series of Fe/Cu-bimetallic organic frameworks (Fe/Cu-MOFs) using simple room-temperature aqueous solvent methods. The pore size structure of Fe/Cu-MOFs is determined by the Fe/Cu ratio employed in the synthesis process. Remarkably, when the Fe/Cu molar ratio was 1:2, the void ratio of Fe/Cu-MOFs increased to 0.7326 cm 3 /g, with a predominant mesoporous structure, and the maximum tetracycline (TC) adsorption capacity exhibited by Fe/Cu-BTC-1/2 was reported at a Q max of 1130.23 mg/g. The adsorption kinetics followed the quasi-second-order kinetic model, and the adsorption isotherms were consistent. The Fe/Cu-BTC-1/2 was effective throughout a wide pH range (6.0–10.0), exhibiting resilience against ionic interference and enabling recycling. The predominant mechanisms of TC adsorption by Fe/Cu-BTC-1/2 include coordination, vacancy filling, and π-π stacking. Thus, our research provides an excellent adsorbent for TC antibiotics and novel insights into the simple synthesis of BMOFs and their application in environmental remediation.

研究领域: 环境科学 · 生物学
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ChemistrySelect · 2024 ·Vol. 10 ·期 1 ·e202405135 · IF 1.9

One-Pot Synthesis of Magnetically Recyclable Fe3o4@Uio-66 Composite with Enhanced Oxytetracycline Adsorption Capacity

Zhanmeng Liu,Mang Lu,Haitao Gan,Jiacheng Li,Guiqing Gao,Manqing Xu,Xianglian Wang

Graphical OTC molecules diffuse to the surface of FU3 to cause film diffusion, and continue to diffuse and fill into large-, medium- and micro-pores of FU3. FU3 can be π─π conjugated and cation─π bonded with the benzene rings and amino groups of OTC. The charged surface of FU3 leads to a strong electrostatic effect in the adsorption process. The doping of Fe 3 O 4 produces structural defects to promote the OTC adsorption. As one of the most stable metal-organic frame materials (MOFs), UiO-66 has attracted extensive attention in the adsorption field. However, the application of UiO-66 is still constrained by the weak electron-hole charge separation capability and the low accessibility of micropores. In this study, the mesoporous defects of UiO-66 were constructed with acetic acid and doped with Fe 3 O 4 to prepare magnetically recyclable Fe 3 O 4 @UiO-66. The doping of Fe 3 O 4 resulted in the formation of denatured mesoporous defects in UiO-66, which was conducive to adsorption oxytetracycline (OTC) in water. The crystal structure and physicochemical characteristics of Fe 3 O 4 @UiO-66 were examined. By using the static adsorption technique, the adsorption characteristics and mechanism of OTC on Fe 3 O 4 @UiO-66 were investigated. The results reveal that Fe 3 O 4 @UiO-66 has an adsorption capacity of 210 mg g −1 and an OTC removal ratio of 84.0%. The pseudo-second-order kinetics, Elovich, and Langmuir isothermal adsorption models were all applicable to the adsorption process. The adsorption process increased entropy and was an endothermic reaction. Solution pH has a little effect on the adsorption performance. This study provides the possibility of one-step synthesis of MOFs that can efficiently adsorb tetracycline antibiotics in water with low cost and excellent recyclability and reusablity.

CAS / MDL: 1317-61-9
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Fabrication of 3D Bi5O7I/BiOIO3 heterojunction material with enhanced photocatalytic activity towards tetracycline antibiotics

Zhijia Zhu,Chenmiao Zhu,Ruiying Yang,Lingfeng Yan,Chunyan Hu,Baojiang Liu

Exploring the efficient and sustainable photocatalysts is the key pot for the improvement of photocatalytic efficiency. In this work, a series of Bi 5 O 7 I/BiOIO 3 composite materials were successfully prepared via a mild hydrothermal method to make layered BiOIO 3 nanosheets uniformly grown in-situ on the smooth surface of Bi 5 O 7 I microrods. The electronic channel at the interface constructed by the in-situ growth could drastically shorten the distance of electron transmission to accelerate the electron transfer. The formation of Bi 5 O 7 I/BiOIO 3 heterojunction was determined via the characterization of the composition and photochemical analysis. Benefited from this structure, the Bi 5 O 7 I/BiOIO 3 with the mass ratio of 1:1 exhibited over 90% efficiency in degradation of 4 different antibiotics after irradiation for 120 min. After that, 5 cycles proved that Bi 5 O 7 I/BiOIO 3 has excellent stability and reusability, which can guarantee the application in the practical process. Finally, the electron migration path and photocatalytic mechanism of the catalyst are inferred base on the capture experiment and ESR test, which proposed that h + and ·O 2 - were the primary active species in the photocatalytic process and confirmed the formation of Z-type heterojunctions between Bi 5 O 7 I and BiOIO 3 . The heterostructure with well-matched band structure enhances the separation and migration of photogenerated charges, which contributes to improve the photocatalytic activity. The design of novel photocatalyst with high efficiency and low-toxicity provides a new approach to achieve full utilization of solar energy and efficient environmental purification.

研究领域: 材料科学 · 环境科学
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