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1.
Talanta ; 281: 126887, 2024 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-39277936

RESUMEN

Herein, the few-layer Ti3C2Tx nanosheets loaded zeolitic imidazolate framework-67 nanoplates (Ti3C2Tx-ZIF-67) with a unique structure has been synthesized by surfactant control method, and then is employed as the core of precursor. A thin layer of polydopamine as the shell of precursor covered Ti3C2Tx-ZIF-67 forms a micro-nano reactor, leading to the confinement carbonization process. Consequently, a novel sensing material that few-layer Ti3C2Tx nanosheets loaded Co nanoparticles coated N-doped carbon (Ti3C2Tx-Co@NC) is obtained for the non-enzymatic determination of glucose. Owing to the impressive structure, the established glucose sensor based on Ti3C2Tx-Co@NC/glassy carbon electrode exhibits 0.5-100.0 µM of linear detection range and 66.8 nM of detection limit, which tends to detect low concentration of glucose. The synergistic few-layer Ti3C2Tx nanosheets, Co nanoparticles and NC are considered through a series of control experiments. First, few-layer Ti3C2Tx nanosheets provide a good transport channel for electron transfer, resulting in the lower steric hindrance. Second, Co nanoparticles provide active centers for the electrochemical detection. Third, N-doped carbon with conductivity and hydrophilia plays the role of stabilizing material structure to prevent the fragmentation of Ti3C2Tx and the agglomeration of Co nanoparticles. Such work proposes a confined strategy to develop MXene-ZIF-67-derived nanocomposite with high-performance structure.

2.
J Environ Manage ; 370: 122589, 2024 Sep 20.
Artículo en Inglés | MEDLINE | ID: mdl-39305879

RESUMEN

ZIF-67 was grown in situ on carbon cloth (CC) using a simple one-step method. The prepared ZIF-67/CC electrodes exhibited excellent CO2 reduction reaction (CO2RR) performance in a dielectric barrier discharge plasma reactor. The highest concentrations of produced formic acid and formaldehyde were 9.16 and 0.068 mmol L-1 at a reaction time of 1 h, respectively. The high performance is related to the unique high aspect ratio structure and pad-like cavity of ZIF-67, which results not only in an increase in the specific surface area for CO2 adsorption but also in the hydrophobicity of the electrode. Unexpectedly, the superoxide radical (·O2-) greatly affects the reduction performance of the electrode. In addition, the ZIF-67/CC electrode maintained good CO2RR performance in the presence of different pollutants, and the production of formic acid and formaldehyde increased to 10.81 and 0.11 mmol L-1 at 1 h with the addition of 10 mg L-1 phenol. This research provides new directions in the field of plasma catalysis.

3.
Heliyon ; 10(17): e36848, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-39281598

RESUMEN

ZIF-67 nanoparticles were synthesized by a simple method at room temperature and used to remove chlortetracycline hydrochloride (CTC) and doxycycline hydrochloride (DOX) from water. ZIF-67 was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), fourier transform infrared spectroscopy (FT-IR), Brunauer-Emmett-Teller (BET) surface area, X-ray photoelectron spectroscopy (XPS), thermogravimetry (TGA) and zeta potential analyzer. The morphology and chemical composition of the synthesized ZIF-67 were characterized. The effects of key parameters such as pH, dosage, temperature, contact time, different initial concentrations and coexisting ions on the adsorption behavior were systematically studied. The results of batch adsorption experiments indicate that the adsorption process conforms to the pseudo-second-order kinetic model and Sips model. At 303K, the removal rates of CTC and DOX at 150 mg/L reached 99.16 % and 97.61 %, and the maximum adsorption capacity of CTC and DOX reached 1411.68 and 1073.28 mg/g, respectively. At the same time, ZIF-67 has excellent stability and reusability. Most importantly, the possible adsorption mechanism is proposed by exploring the changes of SEM, TEM, BET and FT-IR characterization results before and after the reaction, which mainly includes pore filling, electrostatic interaction and π-π interaction. The prepared ZIF-67 has a large specific surface area (1495.967 m2 g-1), achieves a high removal rate within a short time frame, and maintains a high removal rate across a wide pH range. These characteristics make ZIF-67 a potentially promising adsorbent for removing antibiotics from aqueous solutions.

4.
Artículo en Inglés | MEDLINE | ID: mdl-39287959

RESUMEN

Cobalt-based sulfides (CSs) are generally regarded as potentially valuable anode materials for sodium-ion batteries (SIBs) due to their excellent theoretical capacity and natural abundance. Nevertheless, their slow reaction kinetics and poor structural stability restrict the practical application of the materials. In this study, the dual-carbon-confined Se-CoS2@NC@C hollow nanocubes with anion doping are synthesized using ZIF-67 as the substrate by resorcin-formaldehyde (RF) encapsulation and subsequent carbonization and sulfurization/selenization. RF- and ZIF-67-derived dual-carbon skeleton hollow structures with a robust carbon skeleton and abundant internal space minimize cyclic stress, mitigate volume changes and maintain the structural integrity of the material. More importantly, Se doping increases the lattice spacing of CoS2, weakens the strength of Co-S bonds, and modulates the electronic structure around Co atoms, thereby optimizing the adsorption energy of the material. As a result, the hollow nanocubes of Se-CoS2@NC@C demonstrates excellent electrochemical performance as the anode for SIBs, delivering a high reversible capacity of 549.4 mAh g-1 at 0.5 A g-1 after 100 cycles and a superb rate performance (541.1 mAh g-1 at 0.2  A  g-1, and 393.3 mAh g-1 at 5 A g-1). This study proposes a neoteric strategy for synthesizing advanced anodes for SIBs through the synergy of anion doping engineering and dual-carbon confinement strategy.

5.
J Colloid Interface Sci ; 678(Pt C): 120-133, 2024 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-39288573

RESUMEN

In this paper, a 2 dimensional (2D) metal-organic frameworks (MOFs) nanosheets grown on 1D ZIF-67 modified carbon nanofibers (CNFs) was designed and fabricated with a hierarchical heterostructure. The hierarchical 2D/1D MOFs/CCNF offers rich electrochemical active sites and favorable ion/electron diffusion pathways. The synergistic effect of Co, CNFs and MOFs from heterostructures contributes to superb electrochemical activities. Benefiting from the hierarchical heterostructures optimized by the mass ratio of ZIF-67/PAN and CCNF/NiMOF as well as the type of substrates, CCNF-20@MOF showed a specific capacity of 361.50 C g-1 at 0.5 A g-1, whose charge storage mechanism is dominated by diffusion control. Meanwhile, a bamboo-derived carbon material (BBC) was designed in the solid-state asymmetric supercapacitor (CCNF-20@MOF//BBC). The device exhibited an energy density of 38.89 Wh kg-1 at the power density of 800.02 W kg-1 and excellent cycling stability, that exceed many MOFs based devices. Moreover, it could be successfully used for LED light-emitting, demonstrating a good application prospect. This work provides a feasible strategy for the improved performance of MOFs and CNFs based materials in the field of energy storage.

6.
Small ; : e2406693, 2024 Sep 30.
Artículo en Inglés | MEDLINE | ID: mdl-39344581

RESUMEN

Membrane technology exhibits low cost and high efficiency in gas separation. Zeolite-imidazole framework-67 (ZIF-67) membrane shows a theoretically superior performance in H2/CO2 separation, owing to its effective size-sieving pores between H2 and CO2. However, the gas molecules are permeate through a series of consecutive crystal cells of common ZIF-67 polycrystalline membranes, resulting in high transport resistance to the gas permselective transport. To this end, this work employs a contra-diffusion synthesis to construct a honeycomb ZIF-67 (h-ZIF67) crystalline membrane for low-resistance H2/CO2 permselective transport. The controlled growth of h-ZIF67 following the van der Drift theory produces the honeycomb polycrystal with hierarchical channels for low-resistance gas permeation. The prepared membrane with micron-scale thickness still achieves a H2 permeance as high as 1.6 × 10-7 mol m-2 s-1 Pa-1 and a H2/CO2 selectivity of 17, which can be maintained after a long-term operation for the H2/CO2 mixture separation.

7.
Int J Biol Macromol ; 279(Pt 1): 135148, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39214202

RESUMEN

The accumulation of uremic toxins in the human body poses a deadly risk because it causes chronic kidney disease. To increase the effectiveness of hemodialysis and raise the survival rate, these toxins must be effectively removed from the bloodstream. Developing effective materials for removing these dangerous substances requires a thorough understanding of the interactions between an adsorbent and the uremic toxins. Thankfully, metal-organic frameworks (MOFs) have shown considerable promise for the identification and treatment of kidney disorders. Herein, cotton gauze fabrics (CGF) were carboxylated using monochloroacetic acid to produce carboxymethylated cotton gauze fabrics (CM-CGF). CM-CGF was subsequently decorated in situ with zeolitic imidazolate framework-67, resulting in carboxymethylated cotton gauze fabrics-zeolitic imidazolate framework-67 (CM-CGF-ZIF). The CGF, CM-CGF, and CM-CGF-ZIF were evaluated for potential kidney applications by removing uric acid and creatinine from mimic blood. The results showed that CM-CGF-ZIF had the highest adsorption of uric acid and creatinine. The maximum adsorption capacity of uric acid and creatinine was 164 and 222 mg/g for CM-CGF-ZIF, respectively, compared to 45 and 67 mg/g for CGF. CM-CGF-ZIF showed excellent antibacterial activity, good antifungal activity, low cytotoxicity, and a satisfactory level of blood compatibility.

8.
Environ Sci Pollut Res Int ; 31(40): 53424-53436, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-39190248

RESUMEN

This work is primarily focused on overcoming the limitations of polymeric membranes in achieving the balance between permeability and selectivity of the separation performance. The filler, Zeolitic imidazole framework -67 (ZIF-67) nanoparticles were synthesised in cubical morphology using hexadecyltrimethylammonium bromide (CTAB) as a surfactant via the wet-chemical method. The uniform particles with particle sizes ranging between 120-180 nm were incorporated into the polyvinylidene fluoride (PVDF) matrix to fabricate mixed matrix membranes via the phase inversion method. These mixed matrix membranes were systematically characterised to confirm the chemical, structural and morphological properties of the materials and membranes. Furthermore, the membranes showed a 56.5% improvement in their mechanical properties. The results confirm that 5 wt.% ZIF-67/PVDF membrane showed the best separation results compared to its pure counterpart. The permeability of H2 gas was reported to be 1,094,511 Barrer, with selectivities of 3.03 for H2/CO2 and 3.06 for H2/N2. This represents a 210.6% increase in the permeability of H2 gas. These results demonstrate the influence of ZIF-67 loading in the PVDF polymer matrix along with the potential of ZIF-67/PVDF mixed matrix membranes in the field of hydrogen separation and purification.


Asunto(s)
Hidrógeno , Membranas Artificiales , Polivinilos , Zeolitas , Polivinilos/química , Zeolitas/química , Hidrógeno/química , Permeabilidad , Polímeros/química , Imidazoles/química , Polímeros de Fluorocarbono
9.
Adv Sci (Weinh) ; : e2402352, 2024 Aug 19.
Artículo en Inglés | MEDLINE | ID: mdl-39159046

RESUMEN

H2S gas sensors with facile preparation, low detection limits, and high selectivity are crucial for environmental and human health monitoring. However, it is difficult to maintain a high response of H2S gas sensors under high humidity in practical applications. To face this dilemma, a layer-by-layer growth method is applied to in situ prepare a nanostructured Co(CO3)0.5(OH)·0.11H2O/WO3 coated by a hydrophobic hierarchical ZIF-67 as the H2S sensor. This novel composite exhibits excellent humidity immunity without sacrificing the excellent sensitivity and selectivity of H2S. At a low operating temperature of 90 °C, a remarkable response value of 1052.3 to 100 ppm H2S has been achieved, which is 779 and 9.36 times higher than that of pure WO3 and Co(CO3)0.5(OH)·0.11H2O/WO3, respectively. More importantly, an 82.2% relative response value remains at a high humidity of 75%RH. The sensing mechanisms are investigated using gas chromatography-mass spectrometry (GC-MS), which revealed that the reaction products are H2O and SO2. The high humidity immunity and fast response of the Co(CO3)0.5(OH)·0.11H2O@ZIF-67/WO3 demonstrate the layer-by-layer in situ synthesis method holds the potential application for the development of high-performance WO3-based H2S sensors.

10.
ChemSusChem ; : e202401418, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-39146059

RESUMEN

Electrochemical NO3- reduction reaction (NO3RR) represents a green and sustainable way to produce valuable NH3 for both NH3 production and nitrate contaminant removal, and developing efficient, durable, highly selective catalyst is the key. Herein, we report a facile method to fabricate a catalyst composed of ultrafine Cu nanowires (Cu NWs) encapsulated by ZIF67, namely, CuNW@ZIF67, for efficient NH3 electrosynthesis from nitrate. The CuNW@ZIF67 catalyst exhibited excellent catalytic performance toward NO3RR in alkaline electrolyte, manifested by a large NH3 Faradaic efficiency of 93.7% at -0.5 V versus reversible hydrogen electrode (RHE), a high energy efficiency over 30% at -0.7 V, and robust long-term stability. Such intriguing catalytic properties are mainly ascribed to its structural merits and the strong electronic interaction between Cu NWs and ZIF67. DFT calculations revealed that, the Cu site can easily convert NO3- into NO2-, while the Co site plays a critical role in catalyzing the NO2--to-NH3 process. The study can shed light on rational design of efficient, durable, and highly selective catalysts for NO3RR and beyond.

11.
J Colloid Interface Sci ; 677(Pt B): 740-747, 2024 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-39167965

RESUMEN

Zeolitic imidazolate frameworks (ZIFs), a class of promising metal organic frameworks (MOFs) material, display high porosity and chemical/thermal stability. However, there are problems such as few active sites and restricted exposed active areas, which limit the oxygen evolution reaction (OER) performance of catalysts. Here, starting from zeolitic imidazolate framework-67 (ZIF-67), we have successfully synthesized Pt-doped CoFe layered double hydroxide (Pt/CoFe LDH) catalysts for efficient OER catalysis. The obtained Pt/CoFe LDH-4 catalysts provides large surface areas and abundant active sites, which further improves the OER performance. In detail, the Pt/CoFe LDH-4 exhibits a lower overpotential of 263 mV at a current density of 40 mA cm-2, in 1 M KOH solution, the stability of the catalyst exceeds 120 h at this current density, far superior to commercial catalyst RuO2. This study describes a new design idea for synthesis of LDH catalytic materials with low noble metal doping, which broadens the way to the synthesis of robust OER catalysts derived from ZIF-67.

12.
Environ Sci Pollut Res Int ; 31(33): 46038-46051, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38981963

RESUMEN

Heavy metals are highly toxic and nonbiodegradable, posing a serious threat to the water environment and human beings. Therefore, it is crucial to develop a highly efficient adsorbent that is easy to recover and separate for the removal of heavy metals. In this paper, nitrogen-doped magnetic carbon (NC-67) was prepared by carbonization and hydrochloric acid treatment using cobalt-containing MOF (ZIF-67) as precursor. Then, polyaniline (PANI) was grown directly on NC-67 with high specific surface area by in situ polymerization to prepare polyaniline-coated nitrogen-doped magnetic carbon (NC-67@PANI), which was characterized by XRD, SEM, TEM and VSM, etc. and used for the removal of Cr(VI)from wastewater. The experimental results showed that the adsorption process of Cr(VI) by NC-67@PANI was spontaneous and endothermic, which conformed to the pseudo-second-order model and Freundlich adsorption isotherm model. Due to the synergistic effect of adsorption and reduction, the experimental adsorption capacity of NC-67@PANI for Cr(VI) was 410.2 mg/g. NC-67@PANI maintained a removal efficiency of 65.8% for Cr(VI) after five cycles. In addition, NC-67@PANI had good magnetism and was easy to separate under external magnetic field. The excellent adsorption capacity and easy separation characteristics of NC-67@PANI indicate that it is a promising adsorbent for Cr(VI) removal from wastewater.


Asunto(s)
Compuestos de Anilina , Carbono , Cromo , Nitrógeno , Contaminantes Químicos del Agua , Cromo/química , Compuestos de Anilina/química , Contaminantes Químicos del Agua/química , Carbono/química , Adsorción , Nitrógeno/química , Aguas Residuales/química , Purificación del Agua/métodos , Estructuras Metalorgánicas/química , Imidazoles , Zeolitas
13.
ACS Appl Mater Interfaces ; 16(26): 34254-34265, 2024 Jul 03.
Artículo en Inglés | MEDLINE | ID: mdl-38961577

RESUMEN

Hydroquinone (HQ) in wastewater is of great concern, as it is harmful to human health and threatens the ecological environment. However, the existing adsorbents have low adsorption capacity for HQ. To improve the removal of HQ, N,S-codoped activated carbon-ZIF-67 (NSAC-ZIF-67@C) was synthesized in this study by in situ growth of ZIF-67 on N,S-codoped activated carbon (NSAC) and carbonization. The influence of pH, contact time, and initial concentration on the adsorption behaviors of NSAC-ZIF-67@C on HQ were investigated. Owing to the synergistic effect of abundant active sites and well-developed pore structure, the NSAC-ZIF-67@C achieved a prominent adsorption capacity of 962 mg·g-1 and can still retain high adsorption performance after 5 cycles for HQ, which is superior to that of reported other adsorbents. HQ adsorption follows the pseudo-second-order kinetics model (R2 = 0.99999) and the Freundlich isotherm model. X-ray photoelectron spectroscopy (XPS) analysis before and after adsorption as well as density functional theory (DFT) calculation results showed that pyridinic-N-termini were conducive to the π-π interactions and hydrogen-bonding interactions. Therefore, the adsorption mechanisms of NSAC-ZIF-67@C on HQ involve pore filling, electrostatic attraction, π-π interaction, and hydrogen bonding. This study is expected to provide a reference for designing highly effective adsorbents for wastewater treatment.

14.
J Colloid Interface Sci ; 674: 735-744, 2024 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-38950472

RESUMEN

The development of novel materials for electrodes with high energy densities is essential to the advancement of energy storage technologies. In this study, N-doped layered porous carbon with ZIF-67-derived binary CoFe2O4-Fe particles was successfully fabricated by the pyrolysis of an Fe-based chitosan (CS) hydrogel mixed with ZIF-67 particles. Various characterization techniques were employed to assess the performance of the prepared porous CoFe2O4-Fe@NC composite. This composite exhibits excellent performance owing to the effective combination of multivalent CoFe2O4-Fe particles derived from ZIF-67 with N-doped porous carbon substances with a high surface area, which helps to accelerate ion and charge transfer. The specific capacitance of the CoFe2O4-Fe@NC composite carbonized at 700 °C reached 3960.9F/g at 1 A/g. When this composite is combined with activated carbon (AC) to construct an asymmetric supercapacitor (ASC), a density of energy of up to 84.9 W h kg-1 is attained at a power capacity of 291.6 W kg-1. Moreover, this composite maintained a capacitance retention of up to 94.9 % after 10,000 cycles. This work offers new perspectives on high-performance supercapacitors and their applications.

15.
Mikrochim Acta ; 191(8): 469, 2024 Jul 18.
Artículo en Inglés | MEDLINE | ID: mdl-39023564

RESUMEN

Dual-functional nanomaterial electrodes have the capability to satisfy the requirements for both sweat analysis and the hydrogen evolution reaction (HER), thereby enabling the integration of electrochemical sensing and hydrogen production. In this study, ZIF-67 cubes are synthesized on nickel foam (NF), while TiO2 is obtained through an annealing process. Subsequently, the ZIF-67@TiO2/MoS2 nanocomposite is fabricated on nickel foam via a hydrothermal method. This composite material exhibits exceptional photocatalytic properties and is also suitable for the detection of glucose in sweat. The glucose detection range spans from 10 nM to 10 mM with a sensitivity of 7.24 µA mM-1 cm-2 for a signal-to-noise ratio of 3 and a detection limit of 0.43 µM. Moreover, when utilized as a hydrogen evolution electrode, this material demonstrates a current density of 10 mA cm-2 at an overpotential of 118 mV, with a Tafel slope of 73 mV/dec. The synthesis process is both straightforward and economical. This research introduces a novel concept for the design of multifunctional chemical sensors.

16.
J Colloid Interface Sci ; 676: 331-342, 2024 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-39042960

RESUMEN

The selection of highly efficient materials and the construction of advantageous structures are essential for realizing high-performance electrode materials. In this paper, electrode material Cu2S/C@NiMnCe-LDH/CF with excellent morphology and high performance has been successfully designed and prepared by simple hydrothermal and calcination techniques. First, ZIF-67 is loaded on the outer layer of Cu2S rods to obtain core-shell structured Cu2S@ZIF-67 rods, whose ZIF-67 MOF shell is carbonized to obtain Cu2S@C rods. Then, NiMnCe-LDH are epitaxially loaded on the outer layer of Cu2S@C to obtain Cu2S/C@NiMnCe-LDH rods. At a current density of 2 mA cm-2, Cu2S/C@NiMnCe-LDH/CF exhibits an area capacitance of 5176.4 mF cm-2. The mass capacitance and the energy density of the Cu2S/C@NiMnCe-LDH/CF//AC asymmetric supercapacitor (ASC) reach 150.82F g-1 at a sweep rate of 0.8 A/g and 53.62 Wh kg-1 at a power density of 639.99 W kg-1, respectively. Meanwhile, after 8000 electrochemical cycles, the specific capacitance of Cu2S/C@NiMnCe-LDH/CF//AC still has a retention rate of 86.32 %, which proves its excellent cycling stability. These results demonstrate a new strategy for the preparation of novel core-shell structured Cu2S/C@NiMnCe-LDH/CF nanocomposite material for electrode materials of energy storage devices with superb performance.

17.
Molecules ; 29(12)2024 Jun 19.
Artículo en Inglés | MEDLINE | ID: mdl-38930986

RESUMEN

In this study, hybrid skeleton material ZIF-8@ZIF-67 was synthesized by the epitaxial growth method and then was utilized as a carrier for encapsulating Pseudomonas fluorescens lipase (PFL) through the co-precipitation method, resulting in the preparation of immobilized lipase (PFL@ZIF-8@ZIF-67). Subsequently, it was further treated with glutaraldehyde to improve protein immobilization yield. Under optimal immobilization conditions, the specific hydrolytic activity of PFL@ZIF-8@ZIF-67 was 20.4 times higher than that of the free PFL. The prepared biocatalyst was characterized and analyzed by scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transform infrared (FT-IR). Additionally, the thermal stability of PFL@ZIF-8@ZIF-67 at 50 °C was significantly improved compared to the free PFL. After 7 weeks at room temperature, PFL@ZIF-8@ZIF-67 retained 78% of the transesterification activity, while the free enzyme was only 29%. Finally, PFL@ZIF-8@ZIF-67 was applied to the neryl acetate preparation in a solvent-free system, and the yield of neryl acetate reached 99% after 3 h of reaction. After 10 repetitions, the yields of neryl acetate catalyzed by PFL@ZIF-8@ZIF-67 and the free PFL were 80% and 43%, respectively.


Asunto(s)
Enzimas Inmovilizadas , Lipasa , Pseudomonas fluorescens , Enzimas Inmovilizadas/química , Enzimas Inmovilizadas/metabolismo , Pseudomonas fluorescens/enzimología , Lipasa/química , Lipasa/metabolismo , Esterificación , Estabilidad de Enzimas , Zeolitas/química , Espectroscopía Infrarroja por Transformada de Fourier , Temperatura , Acetatos/química , Difracción de Rayos X , Biocatálisis , Imidazoles
18.
Mikrochim Acta ; 191(7): 403, 2024 06 18.
Artículo en Inglés | MEDLINE | ID: mdl-38888689

RESUMEN

An efficient PEC biosensor is proposed for ATP detection based on exciton energy transfer from CdTe quantum dots (CdTe QDs) to Au nanoparticles (AuNPs), integrating CRISPR/Cas12a trans-cleavage activity and specific recognition of ZIF-67 to ATP. Exciton energy transfer between CdTe QDs and AuNPs system is firstly constructed as photoelectrochemical (PEC) sensing substrate. Then, the activator DNAs, used to activate CRISPR/Cas12a, are absorbed on the surface of ZIF-67. In the presence of ATP, the activator DNAs are released due to more efficient adsorption of ZIF-67 to ATP. The released activator DNA activates trans-cleavage activity of CRISPR/Cas12a to degrade ssDNA on the electrode, leading to the recovery of photocurrent due to the interrupted energy transfer. Benefiting from the specific recognition of ZIF-67 to ATP and CRISPR/Cas12a-modulated amplification strategy, the sensor is endowed with excellent specificity and high sensitivity.


Asunto(s)
Adenosina Trifosfato , Técnicas Biosensibles , Sistemas CRISPR-Cas , Compuestos de Cadmio , Técnicas Electroquímicas , Oro , Nanopartículas del Metal , Puntos Cuánticos , Técnicas Biosensibles/métodos , Adenosina Trifosfato/análisis , Adenosina Trifosfato/química , Técnicas Electroquímicas/métodos , Técnicas Electroquímicas/instrumentación , Compuestos de Cadmio/química , Puntos Cuánticos/química , Oro/química , Nanopartículas del Metal/química , Telurio/química , Imidazoles/química , Proteínas Asociadas a CRISPR/química , Límite de Detección , Zeolitas/química , Endodesoxirribonucleasas/química , Estructuras Metalorgánicas/química , Procesos Fotoquímicos , Proteínas Bacterianas/química , Proteínas Bacterianas/genética
19.
ACS Appl Mater Interfaces ; 16(27): 34973-34987, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38918892

RESUMEN

A peroxymonosulfate oxidation system was developed via modification of ß-cyclodextrin (ß-CD) on the surface of Fe2+-doped ZIF-67 (CD/Fe@ZIF-67) as an activator. The 99.7% carbamazepine, 91.3% bisphenol A (BPA), and 95.4% diclofenac (DCF) degradation efficiency were achieved within 10 min, 60, and 1 min, respectively. The hydrophobicity of these three pollutants is positively correlated with their adsorption kinetic constants by CD/Fe@ZIF-67 due to the introduction of ß-CD. Scavenger experiments and electron spin resonance spectra confirmed that carbamazepine was preferentially oxidized by SO4•- [λ(SO4•-)(70.5%) > λ(•OH)(28.2%) > λ(O2•-)(1.3%)], where SO4•- and O2•- played dominant roles in the degradation of BPA [λ(SO4•-)(71.7%) > λ(O2•-)(22.8%) > λ(•OH)(5.5%)], and O2•- was responsible for DCF removal [λ(O2•-) = 93.2%]. Additionally, the particulate catalyst was immobilized in the shell side of a ceramic membrane in a membrane reactor for catalyst recovery. This reactor achieved nearly 100% removal efficiency under optimal conditions: 0.036 wt % catalyst loading, 0.5 mM peroxymonosulfate concentration, 1 L inflow, 10 mg/L initial carbamazepine concentration, and 0.012 L/min hydraulic retention time. In summary, this study elucidates the active role of ß-CD in a polymetallic/peroxymonosulfate system and provides valuable insights into the development of effective oxidation methods for pharmaceutical and personal care products in wastewater.


Asunto(s)
Carbamazepina , Nanocompuestos , Contaminantes Químicos del Agua , beta-Ciclodextrinas , beta-Ciclodextrinas/química , Contaminantes Químicos del Agua/química , Carbamazepina/química , Nanocompuestos/química , Purificación del Agua/métodos , Estructuras Metalorgánicas/química , Compuestos de Bencidrilo/química , Oxidación-Reducción , Fenoles/química , Preparaciones Farmacéuticas/química , Diclofenaco/química , Adsorción , Cosméticos/química , Zeolitas/química , Imidazoles
20.
Food Chem ; 452: 139481, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-38723565

RESUMEN

As a hypertoxic natural toxin, the risk of Microcystin-leucine-arginine (MC-LR) residues in Bellamya aeruginosa deserves more attention. Herein, employing the conventional thin-layer chromatography (TLC) technology and a novel surface-enhanced Raman scattering (SERS) substrate, a TLC-SERS chip was fabricated for the purification and quantitative detection of MC-LR in complex samples. The substrate exhibited excellent SERS performance with an enhancement factor of 6.6 × 107, a low detection limit of 2.27 × 10-9 mM for MC-LR, excellent uniformity and reproducibility, as well as a wide linear range. With the application of TLC, the MC-LR was efficiently purified and the concentration was increased to >3 times. Ultimately, recovery rates fluctuated between 93.28% and 101.66% were obtained from the TLC-SERS chip. On balance, the TLC-SERS chip has a robust capacity for achieving rapid and stable quantitative detection of MC-LR, which promises to improve the efficiency of food safety monitoring.


Asunto(s)
Toxinas Marinas , Microcistinas , Plata , Espectrometría Raman , Microcistinas/análisis , Espectrometría Raman/métodos , Toxinas Marinas/análisis , Cromatografía en Capa Delgada/métodos , Plata/química , Contaminación de Alimentos/análisis , Oro/química , Nanopartículas del Metal/química , Límite de Detección , Imidazoles , Zeolitas
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