JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2025
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IF 4.7
Huihui Su,Zeqian Ren,Peng Chen,Miao Yue,Na Sun,Jianhong Wang,Jizhou Wu,Yongming Fu,Jie Ma
The pervasive presence of antibiotics in natural water bodies has become a critical environmental and health concern. In this work, we have synthesized oxygen-doped graphitic carbon nitride (O-g-C 3 N 4 ) bulk via thermal condensation without any post processing, exhibiting a relatively high specific surface area of 42.053 m 2 g −1 and a reduced band gap to 2.56 eV. The O-g-C 3 N 4 bulk demonstrates the maximum piezo–photocatalytic degradation of ofloxacin (OFL) under blue-light LED irradiation, which perfectly matches with the maximum transmittance wavelength of water, minimizing light absorption loss during propagation in water. Taking advantages of oxygen-doping induced spin-polarization, the O-g-C 3 N 4 bulk achieves nearly complete (99.9 %) degradation of OFL within 12 min under blue-light LED illumination with 50 W power, and the complete degradation time further decreases to 6 min with the assistance of 80 W ultrasonication. The synergistic effect of combining photocatalysis with piezoelectricity is attributed that the ultrasound-induced piezoelectric field facilitates the generation of hydroxyl radicals and improves the separation of photogenerated electron–hole pairs. The findings contribute to sustainable solutions for antibiotic pollution challenges and advance the application of visible light piezo–photocatalysis.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 27
·15340-15353
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IF 3.43
Genxing Zhu,Jialu Zhu,Xinlong Fu,Qi Liu,Fengyi Cao,Yu-nan Li,Qi Qin,Mingli Jiao
In this study, Co nanoparticle-embedded N,O-codoped porous carbon nanospheres (C@Co) with abundant N and O doping, high graphitization, large specific surface area (319 m2 g−1) and a well-developed mesoporous structure were synthesized and characterized thoroughly, and were applied to activate peroxymonosulfate (PMS) for the degradation of methylene blue (MB). Various influential factors affecting the catalytic performance including C@Co dosage, PMS dosage, MB concentration, initial pH, temperature, and co-existing common anions and humic acid (HA) on the MB degradation were systematically investigated. The increase of the C@Co dosage (15–60 mg), PMS dosage (25–100 mg) and reaction temperature (278–308 K) promoted the MB degradation in the C@Co/PMS system. The best performance of the C@Co/PMS system was observed under weakly acidic or nearly neutral conditions. Both the MB concentration (25–100 mg L−1) and Cl− (5–100 mM), NO3− (10–500 mM), CO32− (10–300 mM), HCO3− (1–30 mM) and HA (2–40 mg L−1) had an inhibitory effect on MB degradation, and the degree of decrease in MB degradation increased as their concentrations were enhanced. Interestingly, HPO42− (1–100 mM) had an overall inhibitory effect on the degradation process of MB; however, in comparison with lower concentrations (1–10 mM), an attenuation of the inhibitory effect at higher concentrations (50–100 mM) could be observed. Moreover, the C@Co/PMS system also exhibited general applicability in eliminating various organic pollutants from water such as methyl orange, malachite green, safranine T, Congo red, Rhodamine B, ofloxacin and tetracycline. Classical radical-quenching tests and EPR measurements showed that both the non-radical pathway (major route, involving 1O2) and radical pathway (minor route, involving ˙OH, ˙SO4− and ˙O2−) contribute to the MB degradation. DFT calculations disclosed that the combination of Co–C interactions with graphitic N doping brought in catalytically active sites in C@Co where the charge states of some C atoms were significantly increased. The degradation intermediates of MB during the catalytic reaction were also identified by HPLC-MS and the possible degradation pathway was proposed. Overall, the resultant C@Co can be developed as a novel and efficient heterogeneous catalyst for activating PMS to degrade organic pollutants, and has potential application in environmental remediation.
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ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Jian Song,Hai-Long Qian,Shu-Ting Xu,Cheng Yang,Xiu-Ping Yan
Efficient extraction of perfluoroalkyl and polyfluoroalkyl substances (PFAS) poses a significant challenge for water treatment and food safety. Here, we report a multifunctional covalent organic framework (COF) for the selective and efficient extraction of PFAS. A facile room-temperature imine condensation of two monomers, 2,2′-bis(trifluoromethyl)-4,4′-diaminobiphenyl (BTFDA) and 1,3,5-triformylphloroglucinol (Tp), produced a multifunctional COF (TpBTFDA). TpBTFDA was rationally designed to synergistically integrate chemical moieties capable of leveraging both fluorophilic (via trifluoromethyl groups) and hydrogen bonding (via β-ketoenamine linkages) interactions with PFAS molecules. Batch adsorption experiments, coupled with systematic comparative studies against control COFs (lacking either the fluorophilic or hydrogen-bonding sites), revealed that this synergistic interplay is essential for the efficient capture of PFAS, demonstrating that both interaction mechanisms are indispensable. Consequently, the TpBTFDA exhibited exceptionally high adsorption capacities (379–521 mg g–1) for eight PFAS. The fabricated TpBTFDA was applied to develop a selective solid-phase extraction method for UHPLC-MS/MS determination of PFAS. The developed method showed a wide linear range (0.01–200 μg L–1), low detection limits (0.006–0.59 μg L–1), good precision (RSD ≤ 5.2%), and recovery (83.0–112.3%) for the accurate determination of PFAS in real water and food samples. This study underscores the potential of rationally designed COFs for effectively enriching and detecting PFAS in practical applications.
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Journal of the American Chemical Society
·
2025
·
IF 15.6
Jiaxian Wang,Yunjie Zou,Chengliang Mao,Long Zhao,Ruizhao Wang,Jie Dai,Xingyue Zou,Yan Zhang,Qian Zheng,Bing Zhou,Huan Yang,Yancai Yao,Lizhi Zhang
Efficient defluorination of persistent fluorinated pollutants remains a critical challenge, as conventional oxidant-dependent methods suffer from limited efficacy and poor interference resistance. While enzymatic oxygen transfer defluorination employs high-valent metal-oxo (HVMO) species for selective C–F bond cleavage, replicating this process via an oxidant-free electrochemical synthesis has been elusive. Here, we report an oxidant-free electrochemical platform using low-valent Ir single atoms (+2.0) on titanium foam (L-Ir1/TF) to generate high-valent Ir-oxo (HVIO) species directly from H2O. The higher d-electron count of low-valent Ir enhanced π-backdonation from Ir 5d to O 2p orbitals, concentrating charge density on the axial oxygen. This elevated electrostatic repulsion suppresses competitive *OOH formation, achieving an exceptional HVIO production rate of 16,920 μmol h–1 gIr–1, 1.7 times higher than its high-valent Ir single atom (+4.3) counterpart (H-Ir1/TF). The resultant HVIO species on L-Ir1/TF selectively cleaved C–F bonds via electrophilic addition, achieving 99.4% fluconazole defluorination in 5 h (surpassing H-Ir1/TF by 2.3 times and PbO2 by 6.7 times). This work establishes single-atom oxidation-state engineering as a new paradigm for green HVMO synthesis, enabling the sustainable degradation of recalcitrant fluorinated contaminants.
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DESALINATION
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2025
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IF 9.8
Xin Wang,Yicheng Wang,Xiao Sun,Xiaowen Cui,Tinghui Wu,Ting Wang,Yiran Luo,Yongqi Yang,Mengzhu Liu,Yongpeng Wang,Zhe Chen,Jing Li
Solar-driven interfacial evaporation (SDIE) represents a sustainable pathway for the co-production of freshwater and electricity, offering a promising solution to global water scarcity and energy deficits. However, the development of low-cost, easily fabricated, highly efficient, and salt-resistant water-electricity cogeneration systems remains a significant challenge. Herein, we fabricate a robust and cost-effective 3D solar evaporator (3D-CSC/SA@CF) by integrating corn straw-derived carbon (CSC), discarded cigarette filters (CF), and sodium alginate (SA) hydrogel. In this configuration, the CF scaffold serves as a hydrophilic, quasi-aligned porous substrate for rapid water transport, while the CSC layer functions as an efficient broadband solar absorber, endowing the evaporator with a high light absorption of 97.15 %. Benefiting from its abundant hydrophilic groups and rationally designed porous structure, the evaporation enthalpy is significantly reduced to 851 J g −1 —far below that of pure water. As a result, the evaporator achieves an evaporation rate of 4.52 kg m −2 h −1 under one-sun irradiation (1 kW m −2 , AM 1.5G), with a corresponding solar-to-vapor efficiency of 97.01 %. The system also exhibits remarkable salt-rejection performance, maintaining a stable evaporation rate of 3.22 kg m −2 h −1 in 20 wt% NaCl brine without salt accumulation, and effectively removes heavy metal ions, organic dyes, and antibiotics from simulated wastewater. Furthermore, we construct an integrated thermoelectric cogeneration system based on the evaporator, which delivers a maximum output power density of 307.1 mW m −2 under 1 sun illumination. This work not only demonstrates a sustainable waste-to-resource strategy but also provides a feasible and scalable approach to multifunctional hydro-energy cogeneration, highlighting its potential for practical applications in remote and resource-limited regions.
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ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Jiayue Zhou,Dongmei Li,Ziwei Chen,Tiantian Li,Ying Liu,Jie Nan,Linyuan Wang,Yinuo Chen,Guanggui Yu,Na Sai
Inspired by the color patterns of blue-winged teals’ feathers, a new biomimetic imprinting (IM) probe with chemical fluorescent (CF) color and physical structural (PS) color was developed for the label-free and ratiometric detection of levofloxacin (LOF). The probe is defined by a periodic photonic crystal structure formed by monodisperse imprinting microspheres that incorporate LOF-binding nanocavities, similar to the color emission structure of teals. With the increase of the LOF solution, the probe can selectively bind LOF molecules and demonstrate a two-color response without the use of labels: the CF color emerged from the entering of CF color-emissive LOF molecules, further enhanced by the Purcell effect, while the PS color resulted from the periodic photonic crystal structure. As the concentration of LOF increases, the CF color becomes brighter (turn on), while the PS color becomes darker (turn off). These color changes are perceptible to the naked eye. The probe demonstrated label-free, sensitive (down to 2.77 nmol/L), rapid (10 min), selective, and stable detection of the LOF, utilizing a self-correction function of colors. In addition, the probe was successfully applied in real sample detection.
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TALANTA
·
2025
·
IF 6.1
Mengting Liu,Zuncai Gu,Lu Qian,Kawtar Ettayri,Tao Deng,Chenhao Zhang,Jing Qian,Xingyi Huang,Chengquan Wang
Oxytetracycline (OTC), a broad class of antibacterial medication, has been widely utilized in poultry husbandry and fish farming. However, the presence of OTC residues in the food has become a matter of great concern. These residues have the potential to induce the emergence and spread of bacterial resistance, which can have far-reaching consequences for public health. In this work, we focused on the comparison of the quenching efficiency of UiO-66 and its amino group-modified counterpart UiO-66-NH 2 , towards the fluorescence of nitrogen-doped graphene quantum dots (NGQDs) labeled aptamer (NGQDs-apt). It was found that UiO-66-NH 2 demonstrated a more potent fluorescence quenching ability towards NGQDs-apt, as high as 98.8 %, compared to 69.7 % for UiO-66 without amino functionalization. This enhanced performance is attributed to the improved interaction between the amino groups on UiO-66-NH 2 and the NGQDs-apt, facilitating more effective electron transfer. Consequently, UiO-66-NH 2 was selected as the optimal quencher for the development of a highly sensitive aptasensor. This aptasensor demonstrates a quantitative detection range for OTC spanning from 0.001 to 200 μM with an exceptionally low detection limit of 0.25 nM, showing simplicity, accuracy, stability and great potential for antibiotic residue detection in food samples. This work addresses the urgent need to develop reliable methods for detecting OTC residues in food due to the potential of OTC to trigger bacterial resistance, which is crucial for food safety and public health.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Kaiyue Yang,Pengfei Zhou,Lin Hao,Jinsheng Liang
Solar-driven photodegradation technology is a highly promising route for resolving environmental pollutants. However, the performance of photocatalysts is usually limited by the poor light harvesting, the high recombination of photogenerated electron-hole pairs, and the insufficient surface active sites. In this work, thin Bi 2 O 2 (OH)(NO 3 ) nanosheets co-modified with oxygen vacancies and bromine-grafting (BNSBr-OV) presented a superb rhodamine B photodegradation efficiency of 98.5 % within 4 h under visible light (λ＞420 nm), which was 8.2 times higher than that of pristine Bi 2 O 2 (OH)(NO 3 ). Besides, BNSBr-OV exhibited universal photocatalytic abilities of degrading various antibiotics, including tetracycline hydrochloride, ofloxacin and sodium sulfacetamide. The introduction of oxygen-vacancy and grafted bromine dual active sites can not only improve the light harvesting ability of the photocatalyst, but also promote the migration efficiency of photogenerated carriers, which boosts its photocatalysis performance. This study provides a platform for understanding the dual active sites modified single-crystal material, which potentially offers new design of environmental catalysts for multiple applications.
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JOURNAL OF CHROMATOGRAPHY A
·
2018
·
IF 3.716
Lili Lian,Xinyang Zhang,Jie Hao,Jinyi Lv,Xiyue Wang,Bo Zhu,Dawei Lou
In this study, a unique core-shell titanium-based metal-organic framework (MOF) functionalized magnetic microsphere was constructed and utilized as magnetic adsorbent for enrichment of five fluoroquinolones from water samples. The received magnetic MOF nanocomposite, denoted as Fe 3 O 4 @Cys@MIL125-NH 2 , showed strong magnetic responsiveness, and good hydrophilicity, as well as excellent affinity to the target analytes. Under optimal conditions, the developed magnetic solid-phase extraction (MSPE) method, combined with ultra-high performance liquid chromatography (UPLC), showed good linearity within the studied concentration range, and low limits of detection (0.05-0.2 μg L −1 ). The accuracy of the developed method was evaluated by measuring the extraction recovery of the spiked tap water and river water samples. The satisfactory recoveries of five fluoroquinolones were in the range of 83.8–109.4% with the RSDs lower than 8.9%. These results indicated that the as-prepared Fe 3 O 4 -Cys@MIL125-NH 2 is a promising magnetic adsorbent for efficient enrichment of fluoroquinolones from tap water and environmental water samples.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Guangqian Kuang,Huijuan Cao,Xiangyong Zheng,Yishi Lin,Xingmin Jin,Min Zhao,Wenjuan Han
Antibiotics in wastewater present significant ecological risks. However, their effects on nitrogen (N) removal and greenhouse gas (GHG) emissions in constructed wetlands (CWs) have been largely neglected in previous studies. This study investigated the effects of antibiotics on N removal and GHG emissions in earthworm-enhanced CWs constructed with three earthworm densities (0 g m -2 , 156 g m -2 , and 312 g m -2 ). The results showed that (1) antibiotics significantly increased effluent total inorganic nitrogen (TIN) concentrations by 49.17 % in systems with the high-density earthworm, whereas no significant effects were observed in the other treatments; (2) in systems without earthworms, antibiotics significantly reduced N₂O emissions by 139 %. In systems with low-density earthworms, CH₄ and CO₂ emissions were significantly reduced by 366 % and 70.3 %, respectively. In contrast, in high-density earthworm systems, N₂O emissions significantly increased by 289 %; (3) antibiotics led to a significant reduction in non-CO₂ global warming potential (GWP non-CO₂ , -143 %) in the systems without earthworms and a reduction in total global warming potential (GWP CH₄+N₂O+CO₂ , -57.3 %) in the systems with low-density earthworms. However, both indices significantly increased by 289 % and 51.2 % in systems with high-density earthworms; (4) antibiotics altered the microbial community composition and significantly increased nitrite reductase activity in the systems with low-density earthworms (+24.5 %) but significantly decreased it in systems with high-density earthworms (-33.0 %). In summary, antibiotic contamination markedly influenced both N removal performance and GHG emissions in earthworm-enhanced CWs, with effects varying depending on earthworm density.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Yiheng Yuan,Xishun Peng,Cunwei Wang,Haili Zhang,Caizhen Zu,Zhangyu Zhou,Zhongchen Bai
The threats of antibiotic residues to human health and the environment have become more and more severe due to the overuse of antibiotics in agriculture. Here, multi-walled carbon nanotubes (MWCNTs) were used to prepare MWCNTs@ZnO/Ag substrate by a simple two-step electrochemical deposition process to detect the enrofloxacin (ENR) residues in pork. The coral-like MWCNTs with a large surface area could promote ENR adsorption and provide more sites for growing the ZnO/Ag nanostructures. Moreover, ZnO/Ag nanostructures could not only facilitate the electron transfer to increase Raman intensity but also improve the stability of MWCNTs@ZnO/Ag substrate. Thus, the MWCNTs@ZnO/Ag substrate could easily recognize ENR molecules at a low concentration of 5 × 10 −10 M due to the stronger charge transfer effect between the substrates and analytes. In addition, the limit of detection of ENR residues in pork samples by using MWCNTs@ZnO/Ag substrate was up to 5.87 nM. The SERS sensor of the MWCNTs@ZnO/Ag substrate has a high sensitivity and long-term stability for the detection of antibiotic residues in food, which could be applied in fields of food safety.
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ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Kai Shi,Wenjie Luo,Ying Cheng,Honglei Li,Liai Peng,Xiangrui Luo,Yu Hu,Jiaheng Zhang,Jiaxuan Chen
CRISPR/Cas12a-powered biosensors with guanine (G)-rich sequence reporters (e.g., G-quadruplex and G-triplex) are widely used in detection applications due to their simplicity and sensitivity. However, when these biosensors are employed for molecular detection in complex samples, they may encounter difficulties such as high background signal and susceptibility to interference because of the “turn-off” signal output. Herein, we explore, for the first time, a set of phosphorothioate (ps)-modified G-quadruplex (G4) and G-triplex (G3) sequences that can bind with thioflavin T (ThT) in an active split CRISPR/Cas12a system (SCas12a) to generate a “turn-on” fluorescent signal. To apply this new phenomenon, we develop a universal SCas12a-powered biosensor for “turn-on” fluorescent detection of nucleic acid (miRNA-21) and non-nucleic acid (kanamycin) targets by using ps-modified hairpin G3 as a reporter (SCas12a/psHG3). Target recognition activates SCas12a’s trans-cleavage activity, leading to cleavage at the loop region of the psHG3 reporter. The released prelocked psG3 DNA binds ThT to produce a strong fluorescence signal. Without preamplification, this strategy can detect miRNA-21 with a detection limit of 100 fM. Moreover, the SCas12a/psHG3 system was further utilized for detecting kanamycin by incorporating its aptamers, enabling the detection of kanamycin at concentrations as low as 100 pM. This work is the first to develop a “turn-on” SCas12a/psHG3 system, showcasing its improved performance and wide range of applications in synthetic biology-based sensing technology.
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