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The MAP kinase ERK is important for neuronal plasticity underlying associative learning, yet specific molecular pathways for neuronal ERK activation are undetermined. RapGEF2 is a neuron-specific cAMP sensor that mediates ERK activation. We investigated whether it is required for cAMP-dependent ERK activation leading to other downstream neuronal signaling events occurring during associative learning, and if RapGEF2-dependent signaling impairments affect learned behavior. Camk2α-cre+/-::RapGEF2fl/fl mice with depletion of RapGEF2 in hippocampus and amygdala exhibit impairments in context- and cue-dependent fear conditioning linked to corresponding impairment in Egr1 induction in these two brain regions. Camk2α-cre+/-::RapGEF2fl/fl mice show decreased RapGEF2 expression in CA1 and dentate gyrus associated with abolition of pERK and Egr1, but not of c-Fos induction, following fear conditioning, impaired freezing to context after fear conditioning, and impaired cAMP-dependent long-term potentiation at perforant pathway and Schaffer collateral synapses in hippocampal slices ex vivo. RapGEF2 expression is largely eliminated in basolateral amygdala, also involved in fear memory, in Camk2α-cre+/-::RapGEF2fl/fl mice. Neither Egr1 nor c-fos induction in BLA after fear conditioning, nor cue-dependent fear learning, are affected by ablation of RapGEF2 in BLA. However, Egr1 induction (but not that of c-fos) in BLA is reduced after restraint stress-augmented fear conditioning, as is freezing to cue after restraint stress-augmented fear conditioning, in Camk2α-cre+/-::RapGEF2fl/fl mice. Cyclic AMP-dependent GEFs have been genetically associated as risk factors for schizophrenia, a disorder associated with cognitive deficits. Here we show a functional link between one of them, RapGEF2, and cognitive processes involved in associative learning in amygdala and hippocampus.
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Miedo , Genes Inmediatos-Precoces , Factores de Intercambio de Guanina Nucleótido , Memoria , Transducción de Señal , Animales , Ratones , Proteína 1 de la Respuesta de Crecimiento Precoz/genética , Factores de Intercambio de Guanina Nucleótido/genética , Proteínas Proto-Oncogénicas c-fosRESUMEN
Mixed matrix membranes (MMMs) are one of the most promising solutions for energy-efficient gas separation. However, conventional MMM synthesis methods inevitably lead to poor filler-polymer interfacial compatibility, filler agglomeration, and limited loading. Herein, inspired by symbiotic relationships in nature, we designed a universal bottom-up method for in situ nanosized metal organic framework (MOF) assembly within polymer matrices. Consequently, our method eliminating the traditional postsynthetic step significantly enhanced MOF dispersion, interfacial compatibility, and loading to an unprecedented 67.2 wt % in synthesized MMMs. Utilizing experimental techniques and complementary density functional theory (DFT) simulation, we validated that these enhancements synergistically ameliorated CO2 solubility, which was significantly different from other works where MOF typically promoted gas diffusion. Our approach simultaneously improves CO2 permeability and selectivity, and superior carbon capture performance is maintained even during long-term tests; the mechanical strength is retained even with ultrahigh MOF loadings. This symbiosis-inspired de novo strategy can potentially pave the way for next-generation MMMs that can fully exploit the unique characteristics of both MOFs and matrices.
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We report a systematic analysis of electron beam damage of the zeolitic imidazolate framework (ZIF-8) during liquid cell transmission electron microscopy (LCTEM). Our analysis reveals ZIF-8 morphology is strongly affected by solvent used (water vs dimethylformamide), electron flux applied, and imaging mode (i.e., TEM vs STEM), while ZIF-8 crystallinity is primarily affected by accumulated electron fluence. Our observations indicate that the stability of ZIF-8 morphology is higher in dimethylformamide (DMF) than in water. However, in situ electron diffraction indicates that ZIF-8 nanocrystals lose crystallinity at critical fluence of â¼80 e-Å-2 independent of the presence of solvent. Furthermore, 4D-STEM analysis as a post-mortem method reveals the extent of electron beam damage beyond the imaging area and indicates that radiolytic reactions are more pronounced in TEM mode than in STEM mode. These results illustrate the significance of radiolysis occurring while imaging ZIF-8 and present a workflow for assessing damage in LCTEM experiments.
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Metal-organic frameworks (MOFs) are porous materials with unique characteristics that make them well-suited for drug delivery and gene therapy applications. Among the MOFs, zeolitic imidazolate framework-8 (ZIF-8) has emerged as a promising candidate for delivering exogenous DNA into cells. However, the potential of ZIF-8 as a vector for sperm-mediated gene transfer (SMGT) has not yet been thoroughly explored.This investigation aimed to explore the potential of ZIF-8 as a vector for enhancing genetic transfer and transgenesis rates by delivering exogenous DNA into sperm cells. To test this hypothesis, we employed ZIF-8 to deliver a plasmid expressing green fluorescent protein (GFP) into mouse sperm cells and evaluated the efficiency of DNA uptake. Our findings demonstrate that ZIF-8 can efficiently load and deliver exogenous DNA into mouse sperm cells, increasing GFP expression in vitro. These results suggest that ZIF-8 is a valuable tool for enhancing genetic transfer in SMGT, with important implications for developing genetically modified animals for research and commercial purposes. Additionally, our study highlights the potential of ZIF-8 as a novel class of vectors for gene delivery in reproductive biology.Overall, our study provides a foundation for further research into using ZIF-8 and other MOFs as gene delivery systems in reproductive biology and underscores the potential of these materials as promising vectors for gene therapy and drug delivery.
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The origin of the glass transition is still an open debate, especially for the new class of glasses, formed from metal-organic compounds. High-temperature in situ 2H Nuclear Magnetic Resonance (NMR) experiments are performed on deuterated samples of ZIF-62 (Zn(C3H4N2)2-x(C7H6N2)x, with x = 0.25 and x = 0.05), the prototypical metal-organic framework glass former. Using lineshape analysis, frequencies and angular amplitudes of oscillations of the imidazolate ring during heating up to the melt progressively increasing from ≈10 to 150 MHz, and from ≈5° to 25° are found. This behavior is compositionally dependent and points to the origin of the glass transition lying in organic linker movement, in a similar vein to that witnessed in some organics and contrary to the purely inorganic-based view of Metal-Organic Framework (MOF) glasses taken to date. This experimental approach shows the potential to elucidate the melting and/or decomposition process for a wide range of MOFs.
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To meet the ever-increasing demand of proton exchange membrane fuel cell (PEMFC), it is necessary to carry out structure optimization for low-cost and high-stability oxygen reduction reaction (ORR) catalysts. Herein, a zeolitic imidazolate framework (ZIF)-derived carbon material with a mass of heteroatoms and defects is developed and serves as advanced support for nano-Pt-based ORR catalysts. This unique structure enhances the interaction between nano-Pt and support, leading to higher ORR intrinsic activity. During fuel cell applications, it demonstrates impressive water-retaining capacity and electrochemical stability. Under H2-O2 supply without cathode humidification, this catalyst achieves high mass activity of 0.475 A mgPt -1, with only 7.4% attenuation in maximum power density after 20 000 cycles of accelerated durability test, highlighting its remarkable potential for fuel cell applications. Physicochemical characterization and theoretical simulation reveal the crucial anchoring effect of heteroatom-doped defects to nano-Pt, providing valuable insights for further ORR catalyst design and PEMFC applications.
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Converting hierarchical biomass structure into cutting-edge architecture of electrocatalysts can effectively relieve the extreme dependency of nonrenewable fossil-fuel-resources typically suffering from low cost-effectiveness, scarce supplies, and adverse environmental impacts. A cost-effective cobalt-coordinated nanocellulose (CNF) strategy is reported for realizing a high-performance 2e-ORR electrocatalysts through molecular engineering of hybrid ZIFs-CNF architecture. By a coordination and pyrolysis process, it generates substantial oxygen-capturing active sites within the typically oxygen-insulating cellulose, promoting O2 mass and electron transfer efficiency along the nanostructured Co3O4 anchored with CNF-based biochar. The Co-CNF electrocatalyst exhibits an exceptional H2O2 electrosynthesis efficiency of ≈510.58 mg L-1 cm-2 h-1 with an exceptional superiority over the existing biochar-, or fossil-fuel-derived electrocatalysts. The combination of the electrocatalysts with stainless steel mesh serving as a dual cathode can strongly decompose regular organic pollutants (up to 99.43% removal efficiency by 30 min), showing to be a desirable approach for clean environmental remediation with sustainability, ecological safety, and high-performance.
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Transition metal selenides (TMSs) are receiving considerable interest as improved anode materials for sodium-ion batteries (SIBs) and lithium-ion batteries (LIBs) due to their considerable theoretical capacity and excellent redox reversibility. Herein, ZIF-12 (zeolitic imidazolate framework) structure is used for the synthesis of Cu2Se/Co3Se4@NPC anode material by pyrolysis of ZIF-12/Se mixture. When Cu2Se/Co3Se4@NPC composite is utilized as an anode electrode material in LIB and SIB half cells, the material demonstrates excellent electrochemical performance and remarkable cycle stability with retaining high capacities. In LIB and SIB half cells, the Cu2Se/Co3Se4@NPC anode material shows the ultralong lifespan at 2000 mAg-1, retaining a capacity of 543 mAhg-1 after 750 cycles, and retaining a capacity of 251 mAhg-1 after 200 cycles at 100 mAg-1, respectively. The porous structure of the Cu2Se/Co3Se4@NPC anode material can not only effectively tolerate the volume expansion of the electrode during discharging and charging, but also facilitate the penetration of electrolyte and efficiently prevents the clustering of active particles. In situ X-ray difraction (XRD) analysis results reveal the high potential of Cu2Se/Co3Se4@NPC composite in building efficient LIBs and SIBs due to reversible conversion reactions of Cu2Se/Co3Se4@NPC for lithium-ion and sodium-ion storage.
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In this work, novel ternary composite ZIF-67/Ag NPs/NaYF4:Yb,Er is synthesized by solvothermal method. The photocatalytic activity of the composite is evaluated by sulfadiazine (SDZ) degradation under simulated sunlight. High elimination efficiency of the composite is 95.4% in 180 min with good reusability and stability. The active species (h+, ·O2 - and ·OH) are identified. The attack sites and degradation process of SDZ are deeply investigated based on theoretical calculation and liquid chromatography-mass spectrometry analysis. The upconversion mechanism study shows that favorable photocatalytic effectiveness is attributed to the full utilization of sunlight through the energy transfer upconversion process and fluorescence resonance energy transfer. Additionally, the composite is endowed with outstanding light-absorbing qualities and effective photogenerated electron-hole pair separation thanks to the localized surface plasmon resonance effect of Ag nanoparticles. This work can motivate further design of novel photocatalysts with upconversion luminescence performance, which are applied to the removal of sulphonamide antibiotics in the environment.
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A new method to engineer hierarchically porous zeolitic imidazolate frameworks (ZIFs) through selective ligand removal (SeLiRe) is presented. This innovative approach involves crafting mixed-ligand ZIFs (ML-ZIFs) with varying proportions of 2-aminobenzimidazole (NH2-bIm) and 2-methylimidazole (2-mIm), followed by controlled thermal treatments. This process creates a dual-pore system, incorporating both micropores and additional mesopores, suggesting selective cleavage of metal-ligand coordination bonds. Achieving this delicate balance requires adjustment of heating conditions for each mixed-ligand ratio, enabling the targeted removal of NH2-bIm from a variety of ML-ZIFs while preserving their inherent microporous framework. Furthermore, the distribution of the initial thermolabile ligand plays a pivotal role in determining the resulting mesopore architecture. The efficacy of this methodology is aptly demonstrated through the assessment of hierarchically porous ZIFs for their potential in adsorbing diverse organic dyes in aqueous environments. Particularly striking is the performance of the 10%NH2-ZIF-2 h, which showcases an astonishing 40-fold increase in methylene blue adsorption capacity compared to ZIF-8, attributed to larger pore volumes that accelerate the diffusion of dye molecules to adsorption sites. This versatile technique opens new avenues for designing micro/mesoporous ZIFs, particularly suited for liquid media scenarios necessitating efficient active site access and optimal diffusion kinetics, such as purification, catalysis, and sensing.
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Defect engineering of metal-organic frameworks (MOFs) is a promising strategy for tailoring the interfacial characteristics between MOFs and polymers, aiming to create high-performance mixed matrix membranes (MMMs). This study introduces a new approach using dual defective alkylamine (AA)-modulated zeolitic imidazolate framework-8 (DAZIF-8), to develop high-flux MMMs. Tributylamine (TBA) and triethylamine (TEA) monodentate ligands coordinate with zinc ions in varying compositions. A mixture of Zn(CH3COO)2·2H2O:2-methylimidazole (Mim):AA in a 1:1.75:5 molar ratio facilitates high-yield coordination between Zn and multiple organic ligands, including Zn-Mim, Zn-TEA, and Zn-TBA (>80%). Remarkably, DAZIF-8 containing 3 mol% TBA and 2 mol% TEA exhibits exceptional characteristics, such as a Brunauer-Emmett-Teller surface area of 1745 m2 g-1 and enhanced framework rigidity. Furthermore, dual Zn-AA coordination sites on the framework's outer surface enhance compatibility with the polyimide (PI) matrix through electron donor-acceptor interactions, enabling the fabrication of high-loading MMMs with excellent mechanical durability. Importantly, the PI/DAZIF-8 (60/40 w/w) MMM demonstrates an unprecedented 759% enhancement in ethylene (C2H4) permeability (281 Barrer) with a moderate ethylene/ethane (C2H4/C2H6) selectivity of 2.95 compared to the PI, surpassing the polymeric upper limit for C2H4/C2H6 separation.
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The protection of lead halide perovskite within a stable matrix normally leads to the loss of semiconducting properties. Here, we report the synthesis of perovskite-ZIF glass interpenetrating networks via a cold pressing method, which allows the advantages of bright photoluminescence, high photoconductivity and environmental stability. This hybrid architecture has provided a novel design strategy for the real-world application of perovskite-based devices.
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Core-shell ZIF-8@ZIF-67 was synthesized by growing a cobalt-based ZIF-67 on a ZIF-8 seed particle. Herein, through selective etching of the ZIF-8@ZIF-67 core and subsequent direct carbonization, core-shell hollow ZnO@CoO nitrogen-doped nanoporous carbon (HZnO@CoO-NPC) nanocomposites were prepared. HZnO@CoO-NPCs possessed a high nitrogen content, large surface area, high degree of graphitization and excellent electrical conductivity, all of which were attributed to successfully integrating the unique advantages of ZIF-8 and ZIF-67. HZnO@CoO-NPCs were used to assemble acetylcholinesterase (AChE) biosensors for organophosphorus pesticides (OPs) detection. The low detection limit of 2.74 × 10-13 M for chlorpyrifos and 7.6 × 10-15 M for parathion-methyl demonstrated the superior sensing performance. The results showed that the electrochemical biosensor constructed by HZnO@CoO-NPC provided a sensitive and efficient electrochemical strategy for OPs detection.
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Técnicas Biosensibles , Insecticidas , Metil Paratión , Nanocompuestos , Plaguicidas , Óxido de Zinc , Compuestos Organofosforados , Nitrógeno , Acetilcolinesterasa/química , Técnicas Biosensibles/métodosRESUMEN
Markers of myocardial injury, such as myoglobin (Mb), are substances swiftly released into the peripheral bloodstream upon myocardial cell injury or altered cardiac activity. During the onset of acute myocardial infarction, patients experience a significant surge in serum Mb levels. Given this, precise detection of Mb is essential, necessitating the development of innovative assays to optimize detection capabilities. This study introduces the synthesis of a three-dimensional hierarchical nanocomposite, Cubic-ZIF67@Au-rGOF-NH2, utilizing aminated reduced graphene oxide and zeolite imidazolium ester framework-67 (ZIF67) as foundational structures. Notably, this novel material, applied in a label-free electrochemical immunosensor, presents a groundbreaking approach for detecting myocardial injury markers. Experimental outcomes revealed ZIF67 and AuNPs exhibit enhanced affinity and growth on the 3D-rGOF-NH2 matrix, thus amplifying electrical conductivity while preserving the inherent electrochemical attributes of ZIF67. As a result, the Cubic-ZIF67@Au-rGOF-NH2 label-free electrochemical immunosensor exhibited a broad detection range and high sensitivity for Mb. The derived standard curve was ΔIp = 16.67552lgC+275.245 (R = 0.993) with a detection threshold of 3.47 fg/ml. Moreover, recoveries of standards spiked into samples ranged between 96.3% and 108.7%. Importantly, the devised immunosensor retained notable selectivity against non-target proteins, proving its potential clinical utility based on exemplary sample analysis performance.
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Técnicas Electroquímicas , Oro , Grafito , Estructuras Metalorgánicas , Mioglobina , Mioglobina/análisis , Técnicas Electroquímicas/métodos , Grafito/química , Estructuras Metalorgánicas/química , Oro/química , Humanos , Técnicas Biosensibles/métodos , Nanocompuestos/química , Zeolitas/química , Imidazoles/química , Límite de Detección , Nanopartículas del Metal/químicaRESUMEN
Efficient and robust oxygen reduction reaction (ORR) catalysts are essential for the development of high-performance anion-exchange membrane fuel cells (AEMFC). To enhance the electrochemical performance of metal-organic frameworks of cobalt-based zeolite imidazolium skeleton (ZIF-67), this study reported a novel ZIF-67-4@CNT byin situgrowing carbon nanotubes (CNTs) on the surface of ZIF-67 via a mild two-step pyrolysis/oxidation treatment. The electrochemical results showed that the as-prepared ZIF-67-4@CNT after CTAB modification exhibited excellent catalytic activity with good stability, with Eonset, E1/2, and Ilimit, respectively were 0.98 V (versus RHE), 0.87 V (versus RHE) and 6.04 mA cm-2@1600 rpm, and a current retention rate of about 94.21% after polarized at 0.80 V for 10 000 s, which were all superior to that of the commercial 20 wt% Pt/C. The excellent ORR catalytic performance was mainly attributed to the large amount of thein situgrowing CNTs on the surface, encapsulated with a wide range of valence states of metallic cobalt.
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Due to the misuse and overuse of the antibiotic tetracycline (TC), as well as its refractory degradability, it has become a stubborn environmental contaminant. In this study, a self-standing polyacrylonitrile-based ZIF-67@CNT/ACF aligned anodic membrane was fabricated by innovatively incorporating ZIF-67@CNT nanoparticles into an aligned carbon nanofiber (ACF) membrane to treat the TC. The flow-through nanoporous construction of the ZIF-67@CNT/ACF membrane reactor can compress the diffusion boundary layer on the electrode surface to enhance mass transfer under microscopic laminar flow, which can further enhance the degradation rate. In addition, the enhanced degradation performance also benefited from the significant electrooxidation capacity of the ZIF-67@CNT/ACF membrane. At the optimal electrocatalytic condition of 3.0 V applied potential and pH 6, the degradation rate reached 81% in 1 h for an initial TC concentration of 10 mg l-1. The refractory and highly toxic TC was electrochemically degraded into small non-toxic molecules. Our results indicate that electrocatalytic TC degradation can be enhanced by ZIF-67@CNT/ACF membrane.
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In this study, a sample of 2-methylimidazole zinc salt (ZIF-8) demonstrated high selectivity for the recovery of heavy rare earth elements (REEs) from real rare earth mining wastewater. Results show that the distribution coefficient values of Y3+ (4.02 × 104 mL·g-1), Gd3+ (7.8 × 104 mL·g-1), and Dy3+ (6.8 × 104 mL·g-1) are orders of magnitude higher than those of K+ (359.51 mL·g-1), Mn2+ (266.67 mL·g-1), Ca2+ (396.42 mL·g-1), and Mg2+ (239.48 mL·g-1). Moreover, the desorption efficiency of heavy REEs exceeded 40%. Advanced characterizations and density functional theory (DFT) calculations were utilized to elucidate that the heavy REEs were more likely to bind to the nitrogen atoms of imidazole groups on ZIF-8 compared to non-REEs. Furthermore, the adsorption and desorption of heavy REEs primarily depend on the chemical interaction confirmed by adsorption kinetics, isotherm model, and thermodynamic analysis, which involves the dissociation of water and the formation of REE-O bonds. Finally, the ZIF-8 exhibits a remarkable recovery efficiency of over 40% for heavy REEs in column tests conducted over 7h. The findings reported here provide new insights into the selective recovery of heavy REEs from real mining wastewater.
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Metales de Tierras Raras , Minería , Aguas Residuales , Aguas Residuales/química , Adsorción , Contaminantes Químicos del Agua , Imidazoles/químicaRESUMEN
This study aims to investigate the influence of copper(II) ions as a cofactor on the electrochemical performance of a biocomposite consisting of a mini protein mimicking uricase (mp20) and zeolitic immidazolate framework-8 (ZIF-8) for the detection of uric acid. A central composite design (CCD) was utilized to optimize the independent investigation, including pH, deposition potential, and deposition time, while the current response resulting from the electrocatalytic oxidation of uric acid was used as the response. The statistical analysis of variance (ANOVA) showed a good correlation between the experimental and predicted data, with a residual standard error percentage (RSE%) of less than 2% for predicting optimal conditions. The synergistic effect of the nanoporous ZIF-8 host, Cu(II)-activated mp20, and reduced graphene oxide (rGO) layer resulted in a highly sensitive biosensor with a limit of detection (LOD) of 0.21 µM and a reproducibility of the response (RSD = 0.63%). The Cu(II)-activated mp20@ZIF-8/rGO/SPCE was highly selective in the presence of common interferents, and the fabricated layer exhibited remarkable stability with signal changes below 4.15% after 60 days. The biosensor's reliable performance was confirmed through real sample analyses of human serum and urine, with comparable recovery values to conventional HPLC.
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Cobre , Urato Oxidasa , Humanos , Ácido Úrico/análisis , Reproducibilidad de los Resultados , Técnicas Electroquímicas/métodosRESUMEN
Staphylococcus aureus (S. aureus) is one of the most important pathogens that cause illness and food poisoning. In this research, using a glassy carbon electrode (GCE) modified with zeolite imidazolate framework-8 (ZIF 8) and gold nanoparticles (AuNPs), a sensitive electrochemical aptasensor has been made for the detection of the S. aureus bacteria. The morphology of the prepared AuNPs-ZIF 8 nanocomposite has been carefully characterized by means of transmission electron microscopy (TEM), field emission scanning electron microscopy (FESEM), and energy-dispersive X-ray spectroscopy (EDS). In the manufacturing process, the S. aureus aptamer is immobilized on the AuNPs-ZIF 8 surface. Electrochemical impedance spectroscopy (EIS) method has been used for quantitative determination of S. aureus bacteria. The changes in the charge transfer resistance (Rct) of the aptamer due to the change in the concentration of bacteria are considered as the analytical signals. The proposed aptasensor has linear response in the concentration range of 1.5 × 101 to 1.5 × 107 CFU mL-1 of S. aureus bacteria. The detection limit of the method is 3.4 CFU mL-1. Using the developed aptasensor, it is possible to determine S. aureus bacteria in water and milk samples.
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Aptámeros de Nucleótidos , Técnicas Biosensibles , Nanopartículas del Metal , Infecciones Estafilocócicas , Zeolitas , Humanos , Oro/química , Staphylococcus aureus , Nanopartículas del Metal/química , Aptámeros de Nucleótidos/química , Técnicas Biosensibles/métodos , Técnicas Electroquímicas/métodos , Electrodos , Límite de DetecciónRESUMEN
In this study, ZIF-8 nanoparticles were synthesized using a simple method at room temperature. The ZIF-8 nanoparticles were then characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), BET (Brunauer-Emmett-Teller) specific surface area, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA) and zeta potential. Subsequent batch adsorption experiments evaluated the adsorption performance of ZIF-8 on tetracycline, examining key pa-rameters like reaction time, pH, temperature, and adsorbent dosage. The results revealed a removal rate for TC of up to 90.59%. The adsorption data aligned with the Sips model, showcasing a maximum adsorption capacity of 359.61 mg/g at 303K. Further, the adsorption kinetics adhered to the pseudo-second-order kinetic model with an equilibrium adsorption capacity of 90 mg/g at 303K. The considerable specific surface area of ZIF-8, standing at 1674.169 m2/g, likely enhances the adsorption efficacy. Analysis using XRD and FTIR confirmed the adsorption of TC on the ma-terial's surface. Overall, the predominant driving forces behind the adsorption process were identified as electrostatic interactions and π-π stacking interactions.