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1.
J Hazard Mater ; 473: 134664, 2024 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-38788576

RESUMEN

Epidemiological evidence indicates that exposure to polycyclic aromatic hydrocarbons (PAHs) is associated with certain metabolic diseases. However, the relationship between PAHs and serum lipid profiles in exposed subjects remain unknown. Herein, the associations of multiple (8) urinary hydroxylated PAHs (OH-PAHs) in workers of coking (n = 655) and non-ferrous smelting (n = 614) industries with serum lipid levels (marking lipid metabolism) were examined. Multivariable linear regression, Bayesian kernel machine regression, and quantile g-computation were used. Most urinary OH-PAHs were significantly higher (p < 0.001) in coking workers than in non-ferrous smelting workers. In workers of both industries, OH-PAH exposure was associated with elevated levels of serum total cholesterol, total triglyceride, and low-density lipoprotein, as well as reduced high-density lipoprotein levels. Specifically, urinary 4-hydroxyphenanthrene was significantly positively associated with serum total cholesterol, total triglyceride, and low-density lipoprotein levels in non-ferrous smelting workers; however, the completely opposite association of 4-hydroxyphenanthrene with these lipid levels was observed in coking workers. The results of this pioneering examination suggest that exposure to OH-PAHs may contribute to dyslipidemia in coking and non-ferrous smelting workers, and distinct patterns of change were observed. Further prospective studies involving larger sample sizes are needed to further validate the findings.


Asunto(s)
Coque , Lípidos , Metalurgia , Exposición Profesional , Hidrocarburos Policíclicos Aromáticos , Humanos , Exposición Profesional/análisis , Hidrocarburos Policíclicos Aromáticos/sangre , Hidrocarburos Policíclicos Aromáticos/orina , Adulto , Masculino , Lípidos/sangre , Persona de Mediana Edad , Femenino , Contaminantes Ocupacionales del Aire/sangre , Contaminantes Ocupacionales del Aire/análisis , Contaminantes Ocupacionales del Aire/orina
2.
J Sep Sci ; 47(3): e2300745, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-38356226

RESUMEN

Understanding and comparing the applicability of electromembrane extraction (EME) and liquid-phase microextraction (LPME) is crucial for selecting an appropriate microextraction approach. In this work, EME and LPME based on supported liquid membranes were compared using biological samples, including whole blood, urine, saliva, and liver tissue. After optimization, efficient EME and LPME of clozapine from four biological samples were achieved. EME provided higher recovery and faster mass transfer for blood and liver tissue than LPME. These advantages were attributed to the electric field disrupting clozapine binding to interfering substances. For urine and saliva, EME demonstrated similar recoveries while achieving faster mass transfer rates. Finally, efficient EME and LPME were validated and evaluated combined with liquid chromatography-tandem mass spectrometry (LC-MS/MS). The coefficient of determination of all methods was greater than 0.999, and all methods showed acceptable reproducibility (≤14%), accuracy (90%-110%), and matrix effect (85%-112%). For liver and blood with high viscosity and complex matrices, EME-LC-MS/MS provided better sensitivity than LPME-LC-MS/MS. The above results indicated that both EME and LPME could be used to isolate non-polar basic drugs from different biological samples, although EME demonstrated higher recovery rates for liver tissue and blood.


Asunto(s)
Clozapina , Microextracción en Fase Líquida , Cromatografía Liquida , Reproducibilidad de los Resultados , Espectrometría de Masas en Tándem , Microextracción en Fase Líquida/métodos , Membranas Artificiales
3.
Environ Sci Pollut Res Int ; 31(5): 7828-7836, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-38170364

RESUMEN

Previous works have shown that hematological system can be affected by exposure to lead; however, the effects of multiple metals on platelets remain elusive within the population from metal-contaminated areas. Hence, the study enrolled 609 participants, with 396 from a metal-exposed area and 213 from a control area. Platelet count (PLT), mean platelet volume (MPV), thrombocytocrit (PCT), platelet to large cell ratio (P-LCR), and platelet distribution width (PDW) were selected to evaluate platelet function. Stepwise regression and Lasso regression were utilized to identify the most influential metals. Moreover, the generalized linear model (GLM), Bayesian kernel machine regression (BKMR) models, and quantile g-computation were employed to estimate the individual or combined effects associations between 12 urinary metals and platelet indices. The results revealed all metals except vanadium, copper, strontium, and molybdenum were significantly higher in the exposed group. The GLM models indicated that urinary metals, including lead, antimony, and arsenic, exhibited associations with PLT, MPV, P-LCR, and PDW. Quantile g-computation and BKMR demonstrated negative correlations between metal mixtures and MPV as well as PDW. In conclusion, the study highlights the associations between multiple metal exposures and platelet indices, suggesting that elevated levels of the metal mixture may impede platelet activation in the population in metal-contaminated areas.


Asunto(s)
Plomo , Volúmen Plaquetario Medio , Humanos , Estudios Transversales , Teorema de Bayes , China
4.
J Chromatogr A ; 1714: 464550, 2024 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-38043167

RESUMEN

Molecularly imprinted polymers (MIPs) possess high specific cavities towards the template molecules, thus solid-phase extraction (SPE) based on MIPs using the target as the template has been widely used for selective extraction. However, the performance of SPE depends strongly on the shape and the distribution of the MIP sorbents, and rapid synthesis of MIPs with uniform particles remains a challenge. Our previous studies have shown that reflux precipitation polymerization (RPP) was a simple and rapid method for the synthesis of uniform MIPs. However, synthesis of MIPs by RPP for a group of targets using only one of the targets as the template has rarely been reported. In this work, MIPs with specific recognition capability for a group of quinolone antibiotics were synthesized for the first time via RPP with only ofloxacin as the template. The synthesized MIPs displayed good adsorption performance and selectivity (IF > 3.5) towards five quinolones, and subsequently were used as SPE adsorbents. Based on this MIPs-SPE, after systematic optimization of the SPE operation parameters during loading, washing and elution, an efficient and sensitive enough SPE method for separation and enrichment of the five quinolones in urine was developed and evaluated in combination with LC-MS/MS. The results showed that MIPs-SPE-LC-MS/MS has a good correlation (R2 ≥ 0.9961) in the linear range of 1-500 µg L-1. The limit of detection (LOD) and limit of quantification (LOQ) for the five quinolones were 0.10-0.14 µg L-1 and 0.32-0.48 µg L-1, respectively. In addition, the proposed method demonstrated good reproducibility (≤ 13 %) and high accuracy (92 %-113 %). We are confident that this method holds significant promise for the analysis of quinolones within the contexts of forensic medicine, epidemiology, and environmental chemistry.


Asunto(s)
Impresión Molecular , Quinolonas , Polímeros Impresos Molecularmente , Cromatografía Liquida , Polimerizacion , Reproducibilidad de los Resultados , Impresión Molecular/métodos , Polímeros/química , Espectrometría de Masas en Tándem , Extracción en Fase Sólida/métodos , Antibacterianos , Adsorción
5.
Medicine (Baltimore) ; 102(43): e35507, 2023 Oct 27.
Artículo en Inglés | MEDLINE | ID: mdl-37904467

RESUMEN

Treatment of radial neck fractures (RNFs) in children, particularly those with severe displacement or angulation, remains controversial, largely due to the challenge of achieving optimal reduction without resorting to open reduction. This study aimed to assess the outcomes of ultrasonography (US)-guided percutaneous leverage reduction coupled with US-guided fixation using either elastic stable intramedullary nail (ESIN) or Kirschner wire (KW) for severely displaced Judet type III and IV RNFs in children. We hypothesized that both strategies would be effective and aimed to identify the superior approach. A total of 38 pediatric patients presenting with Judet type III and IV RNFs resulting from falls were treated surgically between January 2020 and January 2022. The cohort comprised 15 boys and 23 girls, aged on average 7.6 ± 2.3 (range: 2.8-11.3 years). The fractures were classified as type III (n = 28) and type IV (n = 10). The patients were divided into 2 treatment groups: ESIN group (n = 15; treated with US-guided percutaneous leverage reduction and ESIN fixation) and the KW group (n = 23; treated with US-guided percutaneous leverage reduction and KW fixation). Variables such as surgical time, frequency of intraoperative radiography, fracture healing time, hospitalization costs, radiographic outcomes, and functional elbow scores were analyzed. Most fractures demonstrated both clinical and radiographic evidence of complete healing within 7 weeks. Based on the Tibone and Stoltz classification (Tibone J, Stoltz M. Fractures of the radial head and neck in children. J Bone Joint Surg Am. 1981;63:100-6), almost all patients had excellent or good clinical outcomes, with only one exception in the ESIN group. The KW group exhibited significantly lower hospitalization costs compared to the ESIN group [(9562.6 vs 12,043.6 + 7694.0)¥, P < .05]. Both groups required notably few intraoperative radiographic exposures (KW: 5.4 ± 2.1 times, ESIN: 4.0 ± 1.9 times, P < .05). No major complications were reported. However, one case of ESIN displacement and joint protrusion was noted. Our study suggests that US-guided percutaneous leverage reduction, combined with either ESIN or KW fixation, is an effective treatment for severely displaced radial neck fractures in children. Both treatment modalities resulted in notably few intraoperative radiographic exposures and yielded favorable clinical and radiological outcomes. The integration of US-guided leverage reduction and KW fixation is both cost-effective and safe.


Asunto(s)
Fijación Intramedular de Fracturas , Fracturas Radiales de Cabeza y Cuello , Fracturas del Radio , Masculino , Femenino , Humanos , Niño , Anciano , Hilos Ortopédicos , Fijación Intramedular de Fracturas/métodos , Clavos Ortopédicos , Resultado del Tratamiento , Fracturas del Radio/diagnóstico por imagen , Fracturas del Radio/cirugía , Fracturas del Radio/etiología , Ultrasonografía , Curación de Fractura , Estudios Retrospectivos , Ultrasonografía Intervencional
6.
Molecules ; 28(20)2023 Oct 15.
Artículo en Inglés | MEDLINE | ID: mdl-37894582

RESUMEN

Molecularly imprinted polymers (MIPs) have gained significant attention as artificial receptors due to their low cost, mild operating conditions, and excellent selectivity. To optimize the synthesis process and enhance the recognition performance, various support materials for molecular imprinting have been explored as a crucial research direction. Yeast, a biological material, offers advantages such as being green and environmentally friendly, low cost, and easy availability, making it a promising supporting substrate in the molecular imprinting process. We focus on the preparation of different types of MIPs involving yeast and elaborate on the specific roles it plays in each case. Additionally, we discuss the advantages and limitations of yeast in the preparation of MIPs and conclude with the challenges and future development trends of yeast in molecular imprinting research.


Asunto(s)
Impresión Molecular , Polímeros Impresos Molecularmente , Saccharomyces cerevisiae , Polímeros/química , Polimerizacion
7.
Artículo en Inglés | MEDLINE | ID: mdl-37725852

RESUMEN

Humans are widely and concurrently exposed to volatile organic compounds (VOCs) and polycyclic aromatic hydrocarbons (PAHs). However, few studies have reported the internal co-exposure levels of these chemicals in occupational and general populations. Specifically, the associations revealed between the urinary levels of metabolites of VOCs (mVOCs), hydroxylated PAHs (OH-PAHs), and oxidative stress biomarkers for humans remain limited. In this study, a method based on solid-phase extraction (SPE) and liquid chromatography coupled with tandem mass spectrometry (LC-MS/MS) was developed for the simultaneous analysis of 22 mVOCs, 12 OH-PAHs, and 8-hydroxy-2'-deoxyguanosine (8-OHdG) in human urine samples. The method was validated with all target analyte accuracies and precisions in the range of 76 %-120 % and 1 %-14 % at three levels of spiked urine samples, respectively. The limit of detection (LOD) and limit of quantification (LOQ) of the target analytes were 0.01-0.34 ng/mL and 0.01-7.57 ng/mL, respectively. And the method was applied to measure urinary levels of target analytes from 38 petrochemical workers in Guangzhou, South China. Except for 3-hydroxy-benzo[a]pyrene, all target analytes were detected in the urine samples. The average levels were 0.05-12.6 ng/mL for individual OH-PAHs, 0.20-73620 ng/mL for individual mVOCs, and 1.00 ng/mL for 8-OHdG. Additionally, 3-hydroxy-phenanthrene, 1-hydroxy-pyrene, 6-hydroxy-chrysene, N-acetyl-S-(trichlorovinyl)-L-cysteine, 2-methylhippuric acid, thiodiacetic acid, trans, trans-Muconic acid, and N-acetyl-S-(3,4-dihydroxybutyl)-L-cysteine had statistically significant positive effects on 8-OHdG levels, while 1-hydroxy-naphthalene, 1,2-dihydroxybenzene, and hippuric acid showed a negative effect on 8-OHdG, indicating these metabolites could lead to synergistic or antagonistic oxidative DNA damage. This study provides a robust analytical method that permits a comprehensive assessment of co-exposure to PAHs and VOCs and their potential adverse health effects.


Asunto(s)
Hidrocarburos Policíclicos Aromáticos , Compuestos Orgánicos Volátiles , Humanos , 8-Hidroxi-2'-Desoxicoguanosina , Hidrocarburos Policíclicos Aromáticos/análisis , Espectrometría de Masas en Tándem/métodos , Cromatografía Líquida de Alta Presión , Cromatografía Liquida/métodos , Cisteína , Biomarcadores/orina
8.
Artículo en Inglés | MEDLINE | ID: mdl-37578923

RESUMEN

Patients with tibial fractures are usually advised to follow a partial weight-bearing gait rehabilitation program after surgery to promote bone healing and lower limb functional recovery. Currently, the biofeedback devices used for gait rehabilitation training in fracture patients use ground reaction force (GRF) as the indicator of tibial load. However, an increasing body of research has shown that monitoring GRF alone cannot objectively reflect the load on the lower limb bones during human movement. In this study, a novel biofeedback system was developed utilizing inertial measurement units and custom instrumented insoles. Based on the data collected from experiments, a hybrid approach combining a physics-based model and neural network architectures was used to predict tibial force. Compared to the traditional physics-based algorithm, the physical guided neural networks method showed better predictive performance. The study also found that regardless of the type of weight-bearing walking, the peak tibial force was significantly higher than the peak tibial GRF, and the time at which the peak tibial compression force occurs may not be consistent with the time at which the peak vertical GRF occurs. This further supports the idea that during gait rehabilitation training for patients with tibial fractures, monitoring and providing feedback on the actual tibial force rather than just the GRF is necessary. The developed device is a non-invasive and reliable portable device that can provide audio feedback, providing a viable solution for gait rehabilitation training outside laboratory and helping to optimize patients' rehabilitation treatment strategies.


Asunto(s)
Fracturas de la Tibia , Dispositivos Electrónicos Vestibles , Humanos , Soporte de Peso Parcial , Caminata , Marcha , Biorretroalimentación Psicológica , Soporte de Peso , Fenómenos Biomecánicos
10.
Mikrochim Acta ; 190(4): 151, 2023 03 23.
Artículo en Inglés | MEDLINE | ID: mdl-36952093

RESUMEN

The development of molecularly imprinted monolith (MIM) for pipette-tip solid-phase extraction (PT-SPE) for sample pretreatment is challenging . In this work, a wax-based molecularly imprinted monolith (WMIM) was successfully prepared with a hybrid method by integration of the traditional packing SPE column and MIM, including preparation of the salt column inside the pipette, polymerization of wax-based imprinted column (WIC) outside the pipette, and immobilization of WIC inside the pipette tip. To ensure the penetration of samples and solvents during the PT-SPE, micrometer-range interconnected macropores were tailor-made via the salt-template sacrifice method. For the production of high affinity imprinted sites within the WIC, octadecanoic acid was used as functional monomer in the paraffin matrix. In terms of the adsorption property, the synthesized WIC exhibited a specific affinity to cardiovascular drugs, with an imprinting factor (IF) of 4.8 for the target analyte. Moreover, the WMIM-based PT-SPE was coupled with fluorescence spectrophotometry for the target propranolol determination  (the excitation and emission wavelengths were 294 nm and 343 nm, respectively). This analytical method showed high recovery of target detection in different real samples (R > 90%), good sensitivity, and accuracy (R2 = 0.99, LOD = 0.03 ng mL-1). We believe this work could provide a significant contribution  for the fabrication of MIM and promote an emerging trend of developing elution-free materials for sample pretreatment.


Asunto(s)
Impresión Molecular , Impresión Molecular/métodos , Polímeros , Cromatografía Líquida de Alta Presión , Extracción en Fase Sólida/métodos , Solventes
11.
Talanta ; 254: 124167, 2023 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-36493567

RESUMEN

Outbreaks of emerging viral respiratory infectious diseases (VRIDs) including coronavirus disease 2019 (COVID-19) seriously endanger people's health. However, the traditional nucleic acid detection required professionals and larger instruments and antigen-antibody detection suffered a long window period of target generation. To facilitate the VRIDs detection in time for common populations, a smartphone-controlled biosensor, which integrated sample preparation (electromembrane extraction), biomarker detection (red-green-blue model) and remote response technology (a built-in APP), was developed in this work. With the intelligent biosensor, VRIDs could be recognized in the early stage by using endogenous hydrogen sulfide as the biomarker. Importantly, it only took 15 min to accomplish the whole process of screening and response to VRIDs. Moreover, the experimental data showed that this smartphone-controlled biosensor was suitable for ordinary residents and could successfully differentiate non-communicable respiratory diseases from VRIDs. To the best of our knowledge, this is the first time that a smartphone-controlled biosensor for screening and response to VRIDs was reported. We believe that the present biosensor will help ordinary residents jointly deal with the challenges brought by COVID-19 or other VRIDs in the future.


Asunto(s)
Técnicas Biosensibles , COVID-19 , Enfermedades Transmisibles , Humanos , Teléfono Inteligente , COVID-19/diagnóstico , COVID-19/epidemiología , Anticuerpos
12.
J Chromatogr A ; 1688: 463738, 2023 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-36574747

RESUMEN

Determination of amphetamine-type drugs (ATSs) in urine and wastewater is a simplified approach for the widespread monitoring of ATSs abuse. To improve the sensitivity of the analytical methods, molecularly imprinted polymers (MIPs) based solid-phase extraction (SPE) pretreatment attracted great attention in this field. Generally, smaller particle sizes and more uniform morphology of the MIPs could provide higher detection sensitivity. Our previous works showed reflux precipitation polymerization (RPP) is a method for synthesizing monodispersed MIPs with small particle size. However, synthesis of uniform spherical MIPs towards a group of targets has never been reported. Therefore, in the present work, MIPs towards a group of ATSs were synthesized via RPP with a pseudo template for the first time. After screening potential pseudo-templates, N-methylphenylethylamine (MPEA) was selected as the optimal pseudo-template. MPEA-MIPs were characterized by scanning electron microscope (SEM), FT-IR spectroscopy and X-ray photoelectron spectroscopy (XPS) spectra. Adsorption isotherms, adsorption kinetics and selectivity were evaluated, and the experimental results indicated that the MPEA-MIPs possessed good selectivity and adsorption property towards ATSs. After optimization of the MIP-SPE procedure, the MIP-SPE cartridges were then coupled with liquid chromatography and tandem mass spectrometry (LC-MS/MS) for determination of ATSs. The evaluation results showed that MIP-SPE-LC-MS/MS displayed good linearity (R2 >0.991) in the linear range (1.0-50.0 µg/L for urine and 0.5-50.0 µg/L for wastewater), and low matrix effect (85-112%). The limit of detection (LOD) was 0.05 -0.29 µg/L, and the accuracy (85-115%) and repeatability (RSD ≤ 15%) were satisfactory at low, medium and high concentrations. To the best of our knowledge, this is the first time that dummy MIPs towards a group of ATSs were synthesized by RPP polymerization, which showed great potential for the detection of ATSs in urine and wastewater.


Asunto(s)
Estimulantes del Sistema Nervioso Central , Impresión Molecular , Anfetamina , Cromatografía Liquida , Polímeros Impresos Molecularmente , Aguas Residuales , Polimerizacion , Espectroscopía Infrarroja por Transformada de Fourier , Polímeros/química , Espectrometría de Masas en Tándem/métodos , Extracción en Fase Sólida/métodos , Impresión Molecular/métodos , Adsorción , Cromatografía Líquida de Alta Presión/métodos
13.
J Hazard Mater ; 443(Pt B): 130254, 2023 02 05.
Artículo en Inglés | MEDLINE | ID: mdl-36356522

RESUMEN

Antibiotic resistance has been a worsening global concern and selective elimination of antibiotic-resistant bacteria (ARB) while retaining the co-existed beneficial bacteria has been essential in environmental protection, which having attracted considerable interest. In this work, by integrating the whole cell imprinting and epitope imprinting strategy, magnetic bacterial imprinted polymers (BIPs) towards ARB were synthesized with interfacial biomimetic mineralization followed by a screening process. The binding data showed that the BIPs owned highly specific affinity towards the target bacteria. Taking advantage of this specific binding ability of BIPs, a two-step selective antimicrobial approach was developed. Remarkably, the BIP nanoantibiotics (nAbts) could efficiently destroy ARB without harming the beneficial bacteria. In comparison with the non-bacterial imprinted polymers, the biocompatible BIP nAbts showed a 12.5-fold increase in the survival percentage for the beneficial bacteria in wastewater. To the best of our knowledge, this is the first time that bacterial imprinting via interfacial biomimetic mineralization was developed, and also the first report of killing ARB without harming the beneficial bacteria in wastewater. We believe that this strategy provides a new insight into the design of novel affinity materials for the selective elimination of ARB in biological treatment for environmental protection.


Asunto(s)
Biomimética , Aguas Residuales , Aguas Residuales/microbiología , Antagonistas de Receptores de Angiotensina , Antibacterianos/farmacología , Inhibidores de la Enzima Convertidora de Angiotensina , Bacterias , Polímeros
14.
Chin J Traumatol ; 26(1): 2-7, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36137934

RESUMEN

Pediatric acute hyperextension spinal cord injury (SCI) named as PAHSCI by us, is a special type of thoracolumbar SCI without radiographic abnormality and highly related to back-bend in dance training, which has been increasingly reported. At present, it has become the leading cause of SCI in children, and brings a heavy social and economic burden. Both domestic and foreign academic institutions and dance education organizations lack a correct understanding of PAHSCI and relevant standards, specifications or guidelines. In order to provide standardized guidance, the expert team formulated this guideline based on the principles of science and practicability, starting from the diagnosis, differential diagnosis, etiology, admission evaluation, treatment, complications and prevention. This guideline puts forward 23 recommendations for 14 related issues.


Asunto(s)
Traumatismos de la Médula Espinal , Niño , Humanos , Traumatismos de la Médula Espinal/diagnóstico , Traumatismos de la Médula Espinal/terapia , Traumatismos de la Médula Espinal/complicaciones , Médula Espinal
15.
Molecules ; 27(21)2022 Oct 29.
Artículo en Inglés | MEDLINE | ID: mdl-36364181

RESUMEN

The separation and detection of flavonoids from various natural products have attracted increasing attention in the field of natural product research and development. Depending on the high specificity of molecularly imprinted polymers (MIPs), MIPs are proposed as efficient adsorbents for the selective extraction and separation of flavonoids from complex samples. At present, a comprehensive review article to summarize the separation and purification of flavonoids using molecular imprinting, and the employment of MIP-based sensors for the detection of flavonoids is still lacking. Here, we reviewed the general preparation methods of MIPs towards flavonoids, including bulk polymerization, precipitation polymerization, surface imprinting and emulsion polymerization. Additionally, a variety of applications of MIPs towards flavonoids are summarized, such as the different forms of MIP-based solid phase extraction (SPE) for the separation of flavonoids, and the MIP-based sensors for the detection of flavonoids. Finally, we discussed the advantages and disadvantages of the current synthetic methods for preparing MIPs of flavonoids and prospected the approaches for detecting flavonoids in the future. The purpose of this review is to provide helpful suggestions for the novel preparation methods of MIPs for the extraction of flavonoids and emerging applications of MIPs for the detection of flavonoids from natural products and biological samples.


Asunto(s)
Productos Biológicos , Impresión Molecular , Flavonoides , Polímeros Impresos Molecularmente , Polímeros , Impresión Molecular/métodos , Extracción en Fase Sólida/métodos
16.
Mikrochim Acta ; 189(9): 324, 2022 08 08.
Artículo en Inglés | MEDLINE | ID: mdl-35939150

RESUMEN

An electromembrane microextraction (EME)-assisted fluorescent molecularly imprinted polymer (MIP) sensing method is presented for detecting the total cathinone drugs in urine samples. In this detection system, the clean-up ability of EME eliminated the matrix effects on both target binding with MIPs and the luminescence of the fluorophore in the sensor. Moreover, by optimizing the extraction conditions of EME, different cathinone drugs with a same concentration show a same response on the single aggregation induced emission (AIE) based MIP (AIE-MIP) sensor (λex = 360 nm, λem = 467 nm). The recoveries were 57.9% for cathinone (CAT) and 78.2% for methcathinone (MCAT). The EME-assisted "light-up" AIE-MIP sensing method displayed excellent performance with a linear range of 2.0-12.0 µmol L-1 and a linear determination coefficient (R2) of 0.99. The limit of detection (LOD) value for EME-assisted "light-up" AIE-MIP sensing method was 0.3 µmol L-1. The relative standard deviation (RSD) values for the detection were found to be within the range 2.0-12.0%. To the best of our knowledge, this is the first time that determination of total illicit drugs with a single fluorescent MIP sensor was achieved and also the first utilization of sample preparation to tune the sensing signal of the sensor to be reported. We believe that this versatile combination of fluorescent MIP sensor and sample preparation can be used as a common protocol for sensing the total amount of a group of analytes in various fields.


Asunto(s)
Alcaloides , Impresión Molecular , Colorantes , Límite de Detección , Impresión Molecular/métodos , Polímeros
17.
Chemosphere ; 304: 135350, 2022 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-35714963

RESUMEN

Pharmaceuticals in hospital effluents, often discharged into the public sewage network without sufficient treatment, have shown negative impacts to the human health and aquatic environment. However, the conventional adsorbents used to remove these micropollutants had several deficiencies, including slow uptake kinetics and poor selectivity. To overcome these challenges, water-compatible Janus MIP particles (J-MIPs) with mouth-like openings were synthesized using seeded interfacial polymerization in this work. Among the series of J-MIPs, the selected J-MIP3 showed fast binding kinetics (∼40 s) towards the target pollutant. The theoretical and instrumental analysis suggested that the electrostatic interaction, hydrogen bond and hydrophobic reaction constituted the dominant mechanism for J-MIP3's recognition of target pharmaceutical. Selectivity and robustness tests indicated that the synthetic method was promising in practical application. Finally, the feasibility of the J-MIP3 fixed-bed column in the rapid removal of propranolol (PRO) from hospital effluents was successfully demonstrated. Compared to the activated carbon fixed-bed column, the J-MIP3 fixed-bed column showed at least 7-fold enhancement in its treatment efficiency. To the best of our knowledge, this is the first time that the accelerated mass transfer and fast removal of the pharmaceutical from wastewater have been achieved by the synthetic receptor with asymmetric structure. We believe the present study will open new avenues for the development of multi-functional molecularly imprinted polymers as well as Janus materials in environmental science.


Asunto(s)
Impresión Molecular , Hospitales , Humanos , Impresión Molecular/métodos , Boca , Preparaciones Farmacéuticas , Polímeros/química , Agua/química
18.
Talanta ; 246: 123485, 2022 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-35462249

RESUMEN

Coextraction of different groups of analytes is vital for saving sample volumes and simplifying analytical procedures in bioanalysis. Conventionally, coextraction was achieved by using multi-extraction systems with different supported liquid membranes (SLMs). However, the different membrane solvents tended to diffuse into the aqueous solutions and the other SLM to reach distribution equilibrium during extraction process, causing the system instability. In this work, a stable multi-extraction system (integration of liquid-phase microextraction and electromembrane extraction, LPME/EME) based on the identical supported semi-liquid membrane (SsLM) was developed. Principally, the state of distribution equilibrium of the membrane solvent (polypropylene glycol with molecular weight 4000) in SsLM could be reached at the beginning of extraction, which enhanced the coextraction stability. With this multi-extraction system, acidic and basic analytes were simultaneously extracted from practical biological samples. The extraction recoveries of the six model drugs in undiluted urine samples were over 70%. Followed by LC-MS/MS, the limits of quantification (LOQs) were in the range of 5-10 ng mL-1. The multi-extraction system using the identical SsLM in this study shows promising potential in construction of other stable multi-extraction systems (e.g., LPME/LPME and EME/EME) in the future, which will greatly benefit the group separation of analytes in complicated biological samples.


Asunto(s)
Microextracción en Fase Líquida , Espectrometría de Masas en Tándem , Cromatografía Liquida , Membranas Artificiales , Solventes
19.
J Mater Chem B ; 10(35): 6742-6751, 2022 09 15.
Artículo en Inglés | MEDLINE | ID: mdl-35377383

RESUMEN

The development of an elution-free solid-phase extraction (SPE) process is of special interest in sample pretreatment. Due to the phase-change merits at relatively low temperatures and easy dissolution in n-hexane, wax spheres show great potential in this field. However, the conventional wax spheres possess a low affinity towards the target analytes when they are used as SPE adsorbents. In this study, using octadecanoic acid as the functional monomer and wax as the matrix, molecularly imprinted wax (MIW) spheres were successfully prepared. The obtained MIW spheres displayed remarkable molecular recognition ability and high selectivity towards the template. Interestingly, the as-synthesized molecularly imprinted wax (MIW) could be dissolved in n-hexane or melted by heating for subsequent fluorescence and mass spectrum analysis without the target elution process. Moreover, the melted MIW exhibited high repeatability, sensitivity and specificity for solid-state fluorescence detection. We believe that the imprinting method presented in this study will open a new window in analytical chemistry.


Asunto(s)
Impresión Molecular , Hexanos , Impresión Molecular/métodos , Extracción en Fase Sólida/métodos
20.
Biosens Bioelectron ; 205: 114113, 2022 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-35219945

RESUMEN

Development of a specific "light-up" sensor for detection of psychoactive drug has been a great challenge in forensic analysis. To achieve this goal, an aggregation induced emission (AIE) functional monomer containing both phenylboronic group and double bond was synthesized for construction of molecularly imprinted polymers (MIPs) based fluorescent sensor. In this AIE-MIP sensor, the AIE fluorophore could vibrate freely in the absence of the target analyte (cathinone, CAT), while this vibration was restricted after the specific molecular recognition, leading to "light-up" character of the corresponding sensor. FT-IR and LC-MS characterizations proved the AIE monomer was successfully introduced onto AIE-MIPs. SEM analysis indicated the AIE-MIPs was ∼140 nm in diameter. Binding experiments indicated the AIE-MIPs owned high specificity towards CAT. Fluorescent studies confirmed that the "light-up" capability of the AIE-MIPs was highly selective. On this basis, the AIE-MIP sensor was applied in detecting CAT in forensic samples. The sensor reached a detection limit of 0.32 µmol L-1 and exhibited a linear range of 2-12 µmol L-1. Compared to previously reported MIPs based electrochemical sensors and fluorescent sensors for measurement of CAT drug and its analogue, the present AIE-MIP sensor showed much higher sensitivity. To the best of our knowledge, this is the first time that an AIE functional monomer was synthesized for molecular imprinting, and also the first "light-up" AIE-MIP sensor to be reported. We believe that this versatile design of the specific "light-up" sensor can be used as a general protocol for construction of advanced sensor in various fields.


Asunto(s)
Técnicas Biosensibles , Impresión Molecular , Impresión Molecular/métodos , Polímeros Impresos Molecularmente , Espectroscopía Infrarroja por Transformada de Fourier
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