CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Tingting Lin,Huajing Zhou,Lingxiang Zhao,Sheng Liang,Yongming Luo,Liang He,Shaoyun Shan,Tianding Hu,Zilian Liu,Wentao Du
The excellent performance of high-valent iron-oxo species (Fe IV O) in the degradation of pollutants by activating peroxymonosulfate (PMS) had attracted much attention. However, the generation and reaction mechanisms were still unclear. In this study, iron-rich paper mill sludge was used as a raw material for the first time to prepare iron-based catalysts with abundant octahedral Fe III sites (Fe oct III ). The results showed that the highest content of Fe oct III was found in the paper mill sludge ash obtained by aerobic calcination at 800 °C ( pm SA800), and the pm SA800 could exhibit excellent catalytic activity (0.4785 min −1 ) and stability during the oxytetracycline (OTC) degradation process. The characterization and density functional theory (DFT) calculations further indicated that the Fe oct III was the dominant active site for Fe IV O production. PMS tended to be adsorbed on two adjacent Fe oct III sites to form a [Fe oct III -OSO 2 OO(H)-Fe oct III ] complex with a two-site adsorption configuration. Subsequently, the O O and O H bonds in [Fe oct III -OSO 2 OO(H)-Fe oct III ] broken by absorbing energy, generating Fe IV O. It's worth noting that the Ca species of pm SA800 effectively stabilized the pH of the reaction solution, which ensured the stable and continuous production of Fe IV O. This work provides a new idea and insight for preparing catalysts that could produce Fe IV O active species.
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ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2025
·Vol. 47
·期 12
·1-21
·
IF 3.8
Yao Runfang,Tao Shiqi,Chen Yuyun,Liu Zengyu,Feng Simin
Antibiotic accumulation in saline-alkaline soils is an escalating problem in agriculture and is receiving increasing attention. Biochar amendment for saline-alkaline land is an effective approach to improve soil quality. However, the effects of modified biochar on the antibiotic adsorption mechanism and occurrence forms in saline-alkaline land remain unclear. In this study, phosphate acid-modified biochar (PBC) was used as the research material, and its effects on the adsorption mechanism, occurrence forms, and bioavailability of oxytetracycline (OTC) in salinized-alkaline soil were investigated. The results showed that the adsorption of OTC by saline-alkali soil amended with 5% PBC reached equilibrium within 24 h, with an adsorption capacity ranging from 2.05 to 4.14 mg/g. The pseudo-second-order kinetic model (R 2 = 0.9754–0.9422) was more suitable for describing this adsorption process, indicating that chemical adsorption dominated. Considering the complex compositions of saline-alkali soil and PBC provided multiple adsorption sites with uneven energy distribution for OTC adsorption (a characteristic of multi-layer adsorption), the Freundlich model (R 2 = 0.9956–0.9634) better fitted the adsorption behavior. PBC effectively reduced the bioavailability of OTC by improving soil properties, including decreasing the pH value of saline-alkali soil, reducing soluble salt content, and increasing organic matter content ( p < 0.01). The bioavailability of OTC decreased by 16.80–25.23% ( p < 0.05) in Na 2 SO 4 saline-alkali soil and by 11.56–15.49% ( p < 0.05) in Na 2 CO 3 saline-alkali soil. The application of PBC in the remediation of OTC-contaminated saline-alkali soil not only enhanced the adsorption capacity for OTC but also improved the physicochemical properties of saline-alkali soil, thereby achieving the synergistic effect of pollution control and soil improvement, as well as effective control of environmental risks.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Meiling Xu,Linchun Nie,Jiawei Liao,Dejing Meng,Wenjing Liu,Haobo Yang,Ranhao Zhao,Qingxiang Zhou
A novel and visible ratiometric fluorescence sensor based on magnesium and nitrogen co-doped carbon dots (Mg, N-CDs) encapsulated in zeolitic imidazolate framework-8 (Mg, N-CDs@ZIF-8) was designed for effective detection of oxytetracycline (OTC), employing a “turn-off/turn-on” fluorescence sensing strategy. The blue-emission Mg, N-CDs@ZIF-8 was quenched owing to fluorescence resonance energy transfer by OTC, while the green fluorescence of OTC was significantly enhanced through the interaction of Mg 2+ and Zn 2+ with OTC, enhancing the visual tracking of OTC through a distinct blue-to-green color transition. This sensor displayed a wide linearity range (0.02 − 25 μg/mL), a low detection limit (14.2 ng/mL), and a fast response time (6 min). The validity of the sensor was successfully verified by detecting OTC in milk, honey, tap water, and lake water samples. Additionally, an expandable fluorescence sensor array was constructed for the discrimination of four tetracycline antibiotics (TCs) in real samples, indicating significant application in complex environmental samples.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yu Liu,Tianyi Hu,Shufei He,Likui Feng,Qingliang Zhao,Junqiu Jiang,Liangliang Wei
Inspired by the high sustainability, energy saving, cleanliness of photocatalysis (PC) with respect to antibiotics decomposition, we developed a stable, highly efficient Bi 2 Ti 2 O 7 @Bi 2 S 3 /polyurethane (BTO@Bi 2 S 3 /PU) photocatalytic system. It exhibited the best degradation performance with the removal of 82.08 % oxytetracycline (OTC) within 180 min under the optimal reaction parameters. Systematic characterization of BTO@Bi 2 S 3 /PU revealed its wider light-harvest capacity, higher electron–hole (e − –h + ) separation efficiency, lower interface resistance, and better redox potential in heterojunction. Based on electrochemical characterization and density functional theory calculation, the construction of Z-scheme BTO@Bi 2 S 3 photocatalyst substantially optimized the band structure. Moreover, the redox cycles of Bi 3+ /Bi 5+ and Ti 4+ /Ti 3+ further enhanced the charge transfer rate during the photoactivation process. For the OTC photodegradation pathways, ·OH, h + , ·O 2 − , and 1 O 2 dominated the pollutant decomposition and the toxicity of intermediates were decreased. Overall, the BTO@Bi 2 S 3 /PU photocatalytic system may provide a universal and stable technique for advanced photoheterojunction applications and wastewater purification.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Peidong Hong,Zijian Wu,Dandan Yang,Kaisheng Zhang,Junyong He,Yulian Li,Chao Xie,Wu Yang,Ya Yang,Lingtao Kong,Jinhuai Liu
Singlet oxygen ( 1 O 2 ) is an electrophilic species that has great selectivity for breaking down electron-rich refractory organic pollutants. However, in most cases, 1 O 2 plays a minor role in the Fenton-like process due to its low yield, the contributions of which are usually covered by free radicals. Here, we provide the first report on a type of hollow amorphous Co/C composites prepared for the efficient generation of 1 O 2 to degrade oxytetracycline (OTC) selectively in the Fenton-like system. The optimized Co/C samples (Co/C-3) obtained the best degradation performance of OTC near to 100% under neutral conditions, along with satisfactory reusability and stability. Additionally, it exhibited a high anti-interference capacity for inorganic anions and natural organic matter s in the different water qualities. XPS spectrum revealed that the electron cycle of ≡Co 2+ -O-C/H and ≡Co 3+ -O-C/H played a vital effect on the formation of 1 O 2 . Quenching experiments and EPR testing further verified that 1 O 2 converted from ·O 2 – was the dominant oxidative species, and no hydroxyl radical (·OH) appeared in this reaction. Moreover, the results of the Fukui function and T.E.S.T (Toxicity Estimation Software Tool) analysis provided significant assistance in the exploration of degradation pathways and ecological risks of OTC and its intermediates.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Chen Liu,Huanxuan Li,Chen Xu,Zijie Shi,Xueheng Wei,Zhitong Yao,Shaodan Xu,Jingang Huang,Mingzhi Huang
The increasing complexity and concentration of refractory organic pollutants in industrial wastewater necessitate the development of efficient and stable advanced oxidation processes (AOPs). Herein, metal–organic framework (MOF)-derived Co₃Fe₇@CN carbon composites were successfully fabricated and evaluated as peroxymonosulfate (PMS) activators for the degradation of oxytetracycline (OTC). Among the as-prepared catalysts, Co₃Fe₇@CN-1 exhibited superior catalytic performance, achieving 90% OTC removal within 10 min with an apparent rate constant ( k obs ) of 0.158 min −1 , which represents a 1.7- and 1.5-fold enhancements over Co₃Fe₇@CN-2 and Co₃Fe₇@CN-3, respectively. The outstanding activity of Co₃Fe₇@CN-1 is primarily attributed to its favorable pore structure and pronounced adsorption–catalysis synergy. Specifically, Co₃Fe₇@CN-1 and Co₃Fe₇@CN-3 achieved 23% and 21% of OTC removal via adsorption, respectively, whereas the dense structure of Co₃Fe₇@CN-2 significantly impeded pollutant uptake (<5%). Mechanistic investigations revealed that PMS activation is driven by the synergistic redox cycling of Co (Co 0 /Co(II)/Co(III)) and Fe (Fe 0 /Fe(II)/Fe(III)) species. Electrons transferred from zero-valent and low-valent metals promote O O bond cleavage in PMS, triggering the generation of SO₄• − and •OH radicals. Crucially, the Fe species acts as an electron reservoir to accelerate the reduction of Co(III) to Co(II), thereby effectively circumventing the rate-limiting step of the Co redox cycle. Simultaneously, high-valent Fe(III)/Co(III) species interact with PMS to form high-valent metal-oxo intermediates ( Fe(IV) O and Co(IV) O), which serve as the predominant reactive species responsible for OTC degradation. The coexistence of radical and non-radical pathways ensures efficient OTC degradation. This work establishes a controllable strategy for constructing MOF-derived carbon catalysts and elucidates the structure–activity relationship between pore architectures and redox centers.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Ming Xie,Yulin Tan,Zhenhua Zhi,Yanfang He,Dawei Cao
Titanium dioxide (TiO 2 ) has been extensively utilized owing to its outstanding physicochemical properties in the field of photocatalytic degradation. However, its efficiency is fundamentally limited by poor charge carrier mobility and severe recombination. These defects critically impair both charge utilization and reactive oxygen species generation. Herein, we in-situ hydrothermally grow ferroelectric barium titanate (BTO) layers on vertically aligned TiO 2 nanorod arrays (NRs), polarize the sample via an external electric field, and load graphene quantum dots (GQDs) through controlled impregnation, successfully constructing a TiO 2 /BTO-Polarized/GQDs (TiO 2 /BTO-P/GQDs) heterostructure. An external electric field induces a stable depolarization field in the BTO layer, creating a persistent interfacial driving force that enhances charge extraction from TiO 2 while suppressing bulk and surface electron-hole recombination. The BTO layer further acts as an electron transfer highway, efficiently channeling photogenerated electrons to GQDs. The π-conjugated system of GQDs serves as both an electron accumulation platform and a chemically active surface, facilitating pollutant adsorption and activation, thereby synergistically accelerating degradation kinetics through combined electron storage and catalytic effects. TiO 2 /BTO-P/GQDs demonstrated a 2.06-fold higher (OTC) degradation efficiency (82.5%) compared to unmodified TiO 2 (40%) within 90 min. This study provides novel insights into ferroelectric polarization-enhanced photocatalytic degradation efficiency. Implication This work presents a highly efficient, stable, and recoverable photocatalyst (TiO 2 /BTO-P/GQDs) for degrading persistent antibiotic pollutants like oxytetracycline in water. By enabling effective solar-driven remediation of agricultural wastewater, it offers a promising strategy to mitigate antibiotic contamination, protect aquatic ecosystems, and reduce risks to microbial communities and human health associated with residual antibiotics in the environment.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Yue-Yang Ma,Ya Li,Hong-Xiang Huang,Dong-Jin Qian
Luminescent lanthanide complexes have attracted growing attention in the visual probe for detection of toxic and dangerous materials. Here, we report an interfacial self-assembly of Eu 3+ -dipicolinic acid complex functionalized nanoSiO 2 composites (nanoSiO 2 PyTAEu) and their Langmuir-Blodgett (LB) films as well as the luminescent probes to tetracycline (TC) and oxytetracycline (OTC). Organic linkers and Eu 3+ ions are anchored on the hydrophilic nanoSiO 2 particles’ surface via the surface silanization, substitution and coordination reactions, so they exhibit high stability and well distribution in the solutions and LB films. Both the nanocomposites of nanoSiO 2 PyTAEu and their LB films show strong and enhanced red fluorescence emissions of Eu 3+ ions when they are immersed in the aqueous TC solution, with the detection limit to 3.3 and 0.91 nmol/L, respectively. The present nanocomposites and LB films have the advantages of high sensitivity and stability.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xuelian Hu,Yichuan Cao,Lin Cai,Haiyang Wang,Guozhen Fang,Shuo Wang
Ultrasensitive and onsite detection of oxytetracycline (OTC) is of vital significance for ensuring public health. Herein, a novel and versatile fluorescence biomimetic nanosensor , Mg,N-CDs@MIL-101@MIP, was elaborately tailored for the assay of OTC. MIL-101 with extraordinarily high surface area and porosity, as a favorable supporter, suppressed self-quenching of Mg,N-CDs and boosted mass transfer rate, realizing signal amplification. As an ultrasensitive signal transducer, high luminescent Mg,N-CDs yielded conspicuous fluorescence responses for OTC, enhancing the sensitivity of Mg,N-CDs@MIL-101@MIP. High-affinity imprinting sites further endowed Mg,N-CDs@MIL-101@MIP with superior anti-interference ability and reusability. Given prominent merits, Mg,N-CDs@MIL-101@MIP demonstrated a good linear range (0.05–40 μg mL −1 ) with a lower limit of detection (16.8 ng mL −1 ), supplying high accessibility to realize ultrasensitive and highly selective measurement of OTC in samples. Additionally, to attain precise onsite profiling of OTC, an intelligent sensing platform was developed by integrating Mg,N-CDs@MIL-101@MIP with a portable smartphone-assisted optical device. As both signal reader and analyzer, smartphone can instantly capture concentration-dependent fluorescent images and accurately digitize them, accomplishing quantitative analysis of OTC. More delightfully, the portable platform was utilized for visual determination of OTC in milk samples with satisfactory results, offering a promising tool for the high-performance onsite evaluation of food safety and environmental health .
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2023
·
IF 4.1
Lin He,Jiabin Zhou,Dan Liu,Yajie Wen,Yuxin Gan
The combination of photocatalysis and Fenton oxidation technology is an efficient strategy to improve the efficiency of oxytetracycline hydrochloride (OTC-HCl) degradation. Herein, a Fe 3 O 4 @GO@MIL-101 composite catalyst bridged with graphene oxide (GO) was obtained by a two-stage hydrothermal method . The introduced graphene oxide layer could inhibit the recombination of electron hole (e − - h + ) pairs by attracting photo-generated electrons from MIL-101 and transferring them to Fe 3 O 4 , observably enhancing the photocatalytic performance of the composite Fe 3 O 4 /MOFs. Under the optimal conditions (initial pH, 10 mmol H 2 O 2 , 0.01 g/L catalyst), the Fe 3 O 4 @GO@MIL-101 + H 2 O 2 +Vis system could achieve a degradation effect of 97.26 % on 70 mg/L OTC-HCl within 50 min Fe 3 O 4 @GO@MIL-101 nanocomposites exhibited good recyclability , were easy to recover after multiple uses, and maintained excellent removal efficiency for pollutants. A series of data demonstrated that in Fe 3 O 4 @GO@MIL-101 + H 2 O 2 +Vis system, the primary active substances involved in OTC-HCl degradation were holes and superoxide radicals , while the contributions of hydroxyl radicals and photo generated electrons were relatively weak. Finally, based on various characterization results and catalyst activity performance, a feasible mechanism for the removal of OTC-HCl by Fenton-like system was proposed.
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CHEMOSPHERE
·
2021
·
IF 7.086
Tingting Yan,Qian Ping,Ai Zhang,Lin Wang,Yicheng Dou,Yongmei Li
In this study, UV-driven advanced oxidation with peracetic acid (PAA) was adopted to enhance the removal of oxytetracycline (OTC) as well as to lower the formation potential of N-nitrosodimethylamine (NDMA). Results implied that the combination of UV and PAA had a synergetic effect on both the removal and mineralization of OTC. OTC (≤5 mg L −1 ) could be completely removed in 45 min in the UV/PAA system under the conditions of an initial pH of 7.10 and a PAA dose of 5 mg L −1 ; additionally, 50.9% of mineralization rate of OTC was obtained. Electron paramagnetic resonance analysis and quenching experiments indicated that ·OH was the main oxidizer for the removal of OTC, while UV, PAA and carbon-centered radicals (R–C·) also participated in its removal. During the degradation of OTC, 31 kinds of degradation intermediates were traced, and 20 kinds of them were first detected in the UV/PAA system. OTC was removed through five pathways, and the hydroxylation pathway was involved in nearly the entire degradation period. The NDMA formation potential decreased by 65.8% after the reaction, and residual dimethylamine accounted for 15.1% of its total composition. The proposed UV/PAA process is a promising method not only for the removal of refractory antibiotics but also for controlling the formation of NDMA.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Yukun Yang,Zhuo Shi,Yuanyuan Chang,Xiaomin Wang,Ligang Yu,Caixia Guo,Jinhua Zhang,Baoqing Bai,Dandan Sun,Sanhong Fan
In order to solve inherent problems of traditional molecularly imprinted electrochemical sensors (MIECS), a novel platform of surface molecularly imprinted magnetic metal-organic frameworks (mMOFs@MIPs) was coupled with magneto electrode to establish magnetic MIECS for the recognition of oxytetracycline (OTC). mMOFs@MIPs were synthesized using layer-by-layer modification method for the recognition of OTC . With the help of magneto electrodes, mMOFs@MIPs can be magnetically modified on the electrode surface, forming the electrochemical sensing interface. The imprinted cavities of mMOFs@MIPs can act as the electron channel of the probe to realize label-free detection of OTC. A linear response was obtained within the OTC concentration range of 1.0 × 10 −9 g mL −1 -1.0 × 10 −4 g mL −1 . The applicability of the sensor was estimated using the spiking and recovery method in milk samples with the recoveries ranging from 89.0% to 103.1%. It has potential applications in food safety analysis with high throughput detection capability, high specificity and good stability.
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