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1.
Sci Rep ; 14(1): 8637, 2024 04 15.
Artigo em Inglês | MEDLINE | ID: mdl-38622241

RESUMO

Rapid mixing and precise timing are key for accurate biomedical assay measurement, particularly when the result is determined as the rate of a reaction: for example rapid immunoassay in which the amount of captured target is kinetically determined; determination of the concentration of an enzyme or enzyme substrate; or as the final stage in any procedure that involves a capture reagent when an enzyme reaction is used as the indicator. Rapid mixing and precise timing are however difficult to achieve in point-of-care devices designed for small sample volumes and fast time to result. By using centrifugal microfluidics and transposing the reaction surface from a chamber to a single mm-scale bead we demonstrate an elegant and easily manufacturable solution. Reagents (which may be, for example, an enzyme, enzyme substrate, antibody or antigen) are immobilised on the surface of a single small bead (typically 1-2 mm in diameter) contained in a cylindrical reaction chamber subjected to periodically changing rotational accelerations which promote both mixing and uniform mass-transfer to the bead surface. The gradient of Euler force across the chamber resulting from rotational acceleration of the disc, dΩdisc/dt, drives circulation of fluid in the chamber. Oscillation of Euler force by oscillation of rotational acceleration with period, T, less than that of the hydrodynamic relaxation time of the fluid, folds the fluid streamlines. Movement of the bead in response to the fluid and the changing rotational acceleration provides a dynamically changing chamber shape, further folding and expanding the fluid. Bead rotation and translation driven by fluid flow and disc motion give uniformity of reaction over the surface. Critical parameters for mixing and reaction uniformity are the ratio of chamber radius to bead radius, rchamber/rbead, and the product Trchamber(dΩdisc/dt), of oscillation period and Euler force gradient across the fluid. We illustrate application of the concept using the reaction of horse radish peroxidase (HRP) immobilised on the bead surface with its substrate tetramethylbenzidine (TMB) in solution. Acceleration from rest to break a hydrophobic valve provided precise timing for TMB contact with the bead. Solution uniformity from reaction on the surface of the bead in volumes 20-50 uL was obtained in times of 2.5 s or less. Accurate measurement of the amount of surface-bound HRP by model fitting to the measured kinetics of colour development at 10 s intervals is demonstrated.


Assuntos
Anticorpos , Microfluídica , Microfluídica/métodos , Antígenos , Sistemas Automatizados de Assistência Junto ao Leito , Interações Hidrofóbicas e Hidrofílicas
2.
Protein Sci ; 33(5): e4986, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38607226

RESUMO

Despite the generally accepted role of the hydrophobic effect as the driving force for folding, many intrinsically disordered proteins (IDPs), including those with hydrophobic content typical of foldable proteins, behave nearly as self-avoiding random walks (SARWs) under physiological conditions. Here, we tested how temperature and ionic conditions influence the dimensions of the N-terminal domain of pertactin (PNt), an IDP with an amino acid composition typical of folded proteins. While PNt contracts somewhat with temperature, it nevertheless remains expanded over 10-58°C, with a Flory exponent, ν, >0.50. Both low and high ionic strength also produce contraction in PNt, but this contraction is mitigated by reducing charge segregation. With 46% glycine and low hydrophobicity, the reduced form of snow flea anti-freeze protein (red-sfAFP) is unaffected by temperature and ionic strength and persists as a near-SARW, ν ~ 0.54, arguing that the thermal contraction of PNt is due to stronger interactions between hydrophobic side chains. Additionally, red-sfAFP is a proxy for the polypeptide backbone, which has been thought to collapse in water. Increasing the glycine segregation in red-sfAFP had minimal effect on ν. Water remained a good solvent even with 21 consecutive glycine residues (ν > 0.5), and red-sfAFP variants lacked stable backbone hydrogen bonds according to hydrogen exchange. Similarly, changing glycine segregation has little impact on ν in other glycine-rich proteins. These findings underscore the generality that many disordered states can be expanded and unstructured, and that the hydrophobic effect alone is insufficient to drive significant chain collapse for typical protein sequences.


Assuntos
Proteínas Intrinsicamente Desordenadas , Dobramento de Proteína , Água/química , Cloreto de Sódio , Glicina/química , Interações Hidrofóbicas e Hidrofílicas
3.
J Agric Food Chem ; 72(15): 8774-8783, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38587054

RESUMO

Proteins can be adsorbed on the air-water interface (AWI), and the structural changes in proteins at the AWI are closely related to the foaming properties of foods and beverages. However, how these structural changes in proteins at the AWI occur is not well understood. We developed a method for the structural assessment of proteins in the foam state using hydrogen/deuterium exchange mass spectrometry. Adsorption sites and structural changes in human serum albumin (HSA) were identified in situ at the peptide-level resolution. The N-terminus and the loop (E492-T506), which contains hydrophobic amino acids, were identified as adsorption sites. Both the structural flexibility and hydrophobicity were considered to be critical factors for the adsorption of HSA at the AWI. Structural changes in HSA were observed after more than one minute of foaming and were spread widely throughout the structure. These structural changes at the foam AWI were reversible.


Assuntos
Proteínas , Albumina Sérica Humana , Humanos , Proteínas/química , Interações Hidrofóbicas e Hidrofílicas , Adsorção , Propriedades de Superfície
4.
ACS Appl Mater Interfaces ; 16(11): 13534-13542, 2024 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-38447594

RESUMO

Prosthetic materials are a source of bacterial infections, with significant morbidity and mortality. Utilizing the bionic "Lotus effect," we generated superhydrophobic vascular prostheses by nanocoating and investigated their resistance to bacterial colonization. Nanoparticles were generated from silicon dioxide (SiO2), and coated vascular prostheses developed a nanoscale roughness with superhydrophobic characteristics. Coated grafts and untreated controls were incubated with different bacterial solutions including heparinized blood under mechanical stress and during artificial perfusion and were analyzed. Bioviability- and toxicity analyses of SiO2 nanoparticles were performed. Diameters of SiO2 nanoparticles ranged between 20 and 180 nm. Coated prostheses showed a water contact angle of > 150° (mean 154 ± 3°) and a mean water roll-off angle of 9° ± 2°. Toxicity and viability experiments demonstrated no toxic effects of SiO2 nanoparticles on human induced pluripotent stem cell-derived cardiomyocytes endothelial cells, fibroblasts, and HEK239T cells. After artificial perfusion with a bacterial solution (Luciferase+ Escherichia coli), bioluminescence imaging measurements showed a significant reduction of bacterial colonization of superhydrophobic material-coated prostheses compared to that of untreated controls. At the final measurement (t = 60 min), a 97% reduction of bacterial colonization was observed with superhydrophobic material-coated prostheses. Superhydrophobic vascular prostheses tremendously reduced bacterial growth. During artificial perfusion, the protective superhydrophobic effects of the vascular grafts could be confirmed using bioluminescence imaging.


Assuntos
Células-Tronco Pluripotentes Induzidas , Dióxido de Silício , Humanos , Dióxido de Silício/farmacologia , Dióxido de Silício/química , Propriedades de Superfície , Biônica , Células Endoteliais , Interações Hidrofóbicas e Hidrofílicas , Água/química , Escherichia coli
5.
Molecules ; 29(6)2024 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-38542857

RESUMO

To produce functional protective textiles with minimal environmental footprints, we developed durable superhydrophobic antimicrobial textiles. These textiles are characterized by a micro-pleated structure on polyester fiber surfaces, achieved through a novel plasma impregnation crosslinking process. This process involved the use of water as the dispersion medium, water-soluble nanosilver monomers for antimicrobial efficacy, fluorine-free polydimethylsiloxane (PDMS) for hydrophobicity, and polyester (PET) fabric as the base material. The altered surface properties of these fabrics were extensively analyzed using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectrometry (XPS), thermogravimetric analysis (TGA), and water contact angle (WCA) measurements. The antimicrobial performance of the strains was evaluated using Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus. After treatment, the fabrics exhibited enhanced hydrophobic and antimicrobial properties, which was attributed to the presence of a micro-pleated structure and nanosilver. The modified textiles demonstrated a static WCA of approximately 154° and an impressive 99.99% inhibition rate against both test microbes. Notably, the WCA remained above 140° even after 500 washing cycles or 3000 friction cycles.


Assuntos
Anti-Infecciosos , Poliésteres , Prata , Poliésteres/química , Têxteis , Anti-Infecciosos/farmacologia , Interações Hidrofóbicas e Hidrofílicas , Água/química
6.
Int J Biol Macromol ; 265(Pt 2): 130994, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38518950

RESUMO

Biofouling remains a persistent challenge within the domains of biomedicine, tissue engineering, marine industry, and membrane separation processes. Multifunctional hydrogels have garnered substantial attention due to their complex three-dimensional architecture, hydrophilicity, biocompatibility, and flexibility. These hydrogels have shown notable advances across various engineering disciplines. The antifouling efficacy of hydrogels typically covers a range of strategies to mitigate or inhibit the adhesion of particulate matter, biological entities, or extraneous pollutants onto their external or internal surfaces. This review provides a comprehensive review of the antifouling properties and applications of hydrogels. We first focus on elucidating the fundamental principles for the inherent resistance of hydrogels to fouling. This is followed by a comprehensive investigation of the methods employed to enhance the antifouling properties enabled by the hydrogels' composition, network structure, conductivity, photothermal properties, release of reactive oxygen species (ROS), and incorporation of silicon and fluorine compounds. Additionally, we explore the emerging prospects of antifouling hydrogels to alleviate the severe challenges posed by surface contamination, membrane separation and wound dressings. The inclusion of detailed mechanistic insights and the judicious selection of antifouling hydrogels are geared toward identifying extant gaps that must be bridged to meet practical requisites while concurrently addressing long-term antifouling applications.


Assuntos
Incrustação Biológica , Hidrogéis , Hidrogéis/farmacologia , Hidrogéis/química , Incrustação Biológica/prevenção & controle , Interações Hidrofóbicas e Hidrofílicas , Silício
7.
Chemosphere ; 355: 141814, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38554862

RESUMO

Evaluating the toxicity of micropollutants forms the basis for understanding their potential risks to the ecosystem and/or human health. To accurately evaluate the toxicity of micropollutants in toxicity tests, many factors have been carefully considered, while the impact of the number of test organisms on toxicity results has rarely been taken into account. In this study, the role of the organism number on the developmental toxicity of five micropollutants was investigated using embryos of the marine polychaete Platynereis dumerilii. The toxicity of hydrophobic micropollutants was found to decrease significantly with increasing the number of embryos used in the test. A quantitative model was developed to better describe how the number of embryos affected developmental toxicity. The model showed a satisfactory fit to the raw data in all scenarios tested. The intrinsic half-maximal effective concentration EC50,int was then determined using the model. For a given compound, the EC50,int was a stable parameter that did not depend on the number of test embryos and thus provided an indication of the intrinsic toxicity of the compounds tested. Compared with the EC50 values determined with the commonly used embryo number (around 120), the EC50,int values of all tested hydrophobic micropollutants were lower. The more hydrophobic the compounds tested, the more pronounced the reduction in toxicity. This suggested that hydrophobic micropollutants could be more toxic than reported in the literature. Some suggestions were also made to eliminate the effect of the number of organisms used in the toxicity evaluation.


Assuntos
Poliquetos , Poluentes Químicos da Água , Animais , Humanos , Ecossistema , Interações Hidrofóbicas e Hidrofílicas , Testes de Toxicidade , Poluentes Químicos da Água/toxicidade
8.
Int J Biol Macromol ; 265(Pt 1): 130650, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38462099

RESUMO

Multifunctional textiles have attracted widespread attention with the improvement of awareness of health. Especially, the fluorine-free superhydrophobic and conductive cellulose fiber-based fabrics have received intensive interest due to their broad and high-value applications. Herein, the copper sulfide nanoflowers were in-situ deposited on cotton fabric followed by polydimethylsiloxane (PDMS) treatment for encapsulating CuS nanoflowers and obtaining superhydrophobicity, recorded as Cot@PTA@CuS@PDMS. Cot@PTA@CuS@PDMS possesses superhydrophobicity with contact angles of 153.0 ± 0.4°, photothermal effect, excellent UV resistance, good conductivity, and anti-fouling. Interestingly, the resistance of Cot@PTA@CuS@PDMS is significantly reduced from 856.4 to 393.1 Ω under simulated sunlight irradiation with 250 mW/cm2. Notably, the resistance can be slightly recovered after shutting off simulated sunlight. Besides, Cot@PTA@CuS@PDMS has efficient oil-water separation efficiency for corn germ oil and castor oil, respectively. Briefly, this work provides a novel, facile, and promising strategy to fabricate multifunctional fiber-based textiles with the reversible change of resistance under simulated sunlight irradiation, inspiring more scholars to control the resistance change of textiles by light irradiation.


Assuntos
Cobre , Têxteis , Dimetilpolisiloxanos , Interações Hidrofóbicas e Hidrofílicas
9.
Int J Biol Macromol ; 265(Pt 1): 130807, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38484808

RESUMO

Magnetic superhydrophobic materials have broad application prospect in oil-water separation. In this study, a magnetic and superhydrophobic aerogel with lamellar structure was successfully prepared using cellulose nanofibrils (CNF) as the skeleton, Fe3O4 as the magnetic ion, 1H, 1H, 2H, 2H trialkylfluorooctane triethoxysilane (FS) and 3-(2-aminoethyl amino)-propyl trimethoxysilane (AS) as the combined modifier. The prepared aerogel shows lower density (38.63 mg/cm3), excellent magnetic (15.13 emu/g), high elasticity and good oil sorption properties (21 g/g). In addition, FS/AS also exhibits excellent mechanical properties and superhydrophobic ability (water contact angle (WCA) of 151.9 ± 1.4°), as it provides sufficient toughness and low surface energy for the layer-branch structure. It should be noted that the entire preparation process is carried out in the aqueous phase, without the use of any organic solvents, providing a green oil-water separation strategy.


Assuntos
Celulose , Água , Elasticidade , Compostos Radiofarmacêuticos , Interações Hidrofóbicas e Hidrofílicas
10.
J Toxicol Sci ; 49(4): 127-137, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38556350

RESUMO

The octanol/water partition coefficient P (logP) is a hydrophobicity index and is one of the determining factors for the pharmacokinetics of orally administered substances because it influences membrane permeability. To illustrate the wide-ranging variety of compounds in the chemical space, a two-dimensional data plot consisting of 25 blocks was previously proposed based on a substance's in silico chemical descriptors. The logP values of approximately 200 diverse chemicals (test plus reference compounds covering all 25 blocks of the chemical space) were estimated experimentally using retention times in reverse-phase liquid chromatography; these values were compared with those of authentic reference compounds with established logP values (available for 17 of 60 reference substances in the Organization for Economic Co-operation and Development Test Guideline 117). The logP values of 140 of 165 chemicals successfully estimated using four different mobile phase conditions (pH 2, 4, 7, and 10 for molecular forms) correlated significantly with those calculated using the in silico packages ChemDraw and ACD/Percepta (r > 0.72). Although substances that neighbored authentic compounds in the chemical space had precisely correlated logP values estimated experimentally and in silico, some compounds that were more distant from authentic substances showed lower logP values than those estimated in silico. These results indicate that additional authentic reference materials with wider ranging chemical diversity and their logP values from reverse-phase liquid chromatography should be included in the international test guidance to promote simple and reliable estimation of octanol/water partition coefficients, which are important determinant factors for the pharmacokinetics of general chemicals.


Assuntos
Cromatografia de Fase Reversa , Água , Cromatografia de Fase Reversa/métodos , Água/química , Octanóis/química , Interações Hidrofóbicas e Hidrofílicas , Cromatografia Líquida de Alta Pressão/métodos
11.
Int J Mol Sci ; 25(6)2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38542241

RESUMO

As the population ages, the number of patients undergoing total hip arthroplasty (THA) and total knee arthroplasty (TKA) continues to increase. Infections after primary arthroplasty are rare but have high rates of morbidity and mortality, as well as enormous financial implications for healthcare systems. Numerous methods including the use of superhydrophobic coatings, the incorporation of antibacterial agents, and the application of topographical treatments have been developed to reduce bacterial attachment to medical devices. However, most of these methods require complex manufacturing processes. Thus, the main purpose of this study was to apply biocoatings to titanium (Ti) surfaces to increase their infection resistance and osteoconductivity via simple processes, without organic reagents. We modified titanium surfaces with a combination of aminomalononitrile (AMN) and an antibiotic-loaded mesoporous bioactive glass (MBG) and evaluated both the antibacterial effects of the coating layer and its effect on osteoblast proliferation and differentiation. The properties of the modified surface, such as the hydrophilicity, roughness, and surface morphology, were characterized via contact angle measurements, atomic force microscopy, and scanning electron microscopy. The cell proliferation reagent WST-1 assay and the alkaline phosphatase (ALP) assay were used to determine the degrees of adhesion and differentiation, respectively, of the MG-63 osteoblast-like cells on the surface. Antimicrobial activity was evaluated by examining the survival rate and inhibition zone of Escherichia coli (E. coli). The AMN coating layer reduced the water contact angle (WCA) of the titanium surface from 87° ± 2.5° to 53° ± 2.3° and this change was retained even after immersion in deionized water for five weeks, demonstrating the stability of the AMN coating. Compared with nontreated titanium and polydopamine (PDA) coating layers, the AMN surface coating increased MG-63 cell attachment, spreading, and early ALP expression; reduced E. coli adhesion; and increased the percentage of dead bacteria. In addition, the AMN coating served as an adhesion layer for the subsequent deposition of MBG-containing antibiotic nanoparticles. The synergistic effects of the AMN layer and antibiotics released from the MBG resulted in an obvious E. coli inhibition zone that was not observed in the nontreated titanium group.


Assuntos
Escherichia coli , Titânio , Humanos , Titânio/farmacologia , Titânio/química , Propriedades de Superfície , Antibacterianos/farmacologia , Antibacterianos/química , Interações Hidrofóbicas e Hidrofílicas , Bactérias , Materiais Revestidos Biocompatíveis/farmacologia , Materiais Revestidos Biocompatíveis/química , Osteoblastos
12.
J Chromatogr A ; 1720: 464780, 2024 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-38458138

RESUMO

In this work, a chromatographic method for the separation of carbohydrates was proposed. Tris-(hydroxymethyl)-amine (TRIS) functionalized silica-based hydrophilic interaction liquid chromatography (HILIC) stationary was synthesized. The dynamically absorbed borate layer is generated by using borate buffer as a polar modifier due to the complexation of borate with TRIS ligand in the stationary phase. The chromatographic systems were analyzed by the linear solvation energy relationship model. The calculated system constants revealed the enhancement of anionic exchange by the addition of borate in the mobile phase system. In addition, ligand exchange is critical for the retention and elution order of sugars and sugar alcohols. Carbohydrates displayed prolonged retention with different selectivity profiles relating to their complexation coefficients with borate. Experiment results showed that the effect of borate in this chromatographic system was stable within the range of pH 3-7 and borate concentration of 5-15 mM. This work provides a complementary solution for the separation of carbohydrates. It can also be extended to the separation of glycosides.


Assuntos
Boratos , Carboidratos , Ligantes , Cromatografia Líquida/métodos , Carboidratos/química , Interações Hidrofóbicas e Hidrofílicas
13.
Plant Physiol Biochem ; 208: 108485, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38461755

RESUMO

Duckweed, a floating macrophyte, has attracted interest in various fields such as animal feedstocks and bioenergy productions. Its enriched nutritional content and rapid growth rate make it particularly promising. However, common laboratory cultures of duckweed often experience fronds layering, diminishing the efficiency of sunlight capturing due to limited surface area on conventional cultivation platforms. In this work, we aimed to address the issue of fronds layering by introducing a novel cultivation platform - a superhydrophobic coated acrylic sheet. The sheet was prepared by spray-coating a suspension of beeswax and ethanol, and its effectiveness was evaluated by comparing the growth performance of giant duckweed, Spirodela polyrhiza, on this platform with that on a modified version. The superhydrophobic coated acrylic sheet (SHPA) and its variant with a metal mesh added (SHPAM) were employed as growing platforms, with a glass jar serving as the control. The plantlets were grown for 7 days with similar growth conditions under low light stress (25 µmol/m2/s). SHPAM demonstrated superior growth performance, achieving a mass gain of 102.12 ± 17.18 %, surpassing both SHPA (89.67 ± 14.97 %) and the control (39.26 ± 8.94 %). For biochemical compositions, SHPAM outperformed in chlorophyll content, protein content and lipid content. The values obtained were 1.021 ± 0.076 mg/g FW, 14.59 ± 0.58 % DW and 6.21 ± 0.75 % DW respectively. Therefore, this work proved that incorporation of superhydrophobic coatings on a novel cultivation platform significantly enhanced the biomass production of S. polyrhiza. Simultaneously, the biochemical compositions of the duckweeds were well-maintained, showcasing the potential of this approach for optimized duckweed cultivation.


Assuntos
Araceae , Luz , Animais , Biomassa , Interações Hidrofóbicas e Hidrofílicas
14.
Sci Total Environ ; 925: 171726, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38492591

RESUMO

Polycyclic aromatic hydrocarbons (PAHs), a group of seriously hazardous environmental contaminants, have attracted extensive attention due to their carcinogenicity, genotoxicity, mutagenicity, and ubiquity. In this work, the excellent hydrophobic trifluoromethyl-enriched covalent organic framework (CF3-COF) was designed and synthesized as coating of solid-phase microextraction (SPME). The CF3-COF offered a high adsorption selectivity for PAHs, which could be attributed to the multiple interactions between the CF3-COF and PAHs, including hydrophobicity interaction, π-π and H bond interactions. Furthermore, headspace (HS) and direct immersion (DI) dual-mode solid-phase microextraction (HS/DI-SPME) were innovatively integrated as a dual-mode extraction by varying the length of SPME coating on stainless-steel, which could simultaneously and efficiently extract 16 PAHs with different volatile. Amazingly, the proposed strategy achieved fast adsorption for PAHs and shortened the adsorption equilibrium time to 15 min. By further integrating with gas chromatography tandem mass spectrometry (GC-MS/MS), PAHs could be detected in the range of 0.008-0.16 ng mL-1 with a quantitative limit of 0.029-0.47 ng mL-1, respectively. The recoveries of PAHs in water samples ranged from 80.84 to 117.67 %. This work indicates that the dual-mode CF3-COF-SPME is a promising candidate for the enrichment of multiple hazardous substances in complicated samples.


Assuntos
Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Hidrocarbonetos Policíclicos Aromáticos/análise , Microextração em Fase Sólida/métodos , Espectrometria de Massas em Tandem , Cromatografia Gasosa-Espectrometria de Massas , Poluentes Químicos da Água/análise , Limite de Detecção , Interações Hidrofóbicas e Hidrofílicas , Água/química
15.
J Chromatogr A ; 1720: 464820, 2024 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-38507872

RESUMO

Highly polar low molecular weight organic molecules are still very challenging to analyze by liquid chromatography. Yet, with the steadily increasing application of metabolomics and similar approaches in chemical analysis, separating polar compounds might be even more important. However, almost all established liquid chromatography techniques (i.e., normal and reversed phase, hydrophilic interaction liquid chromatography (HILIC), ion chromatography) struggle with either carry-over, low sensitivity, or a lack of retention. For improving these shortcomings, electrostatic repulsion hydrophilic interaction chromatography (ERLIC) might be an alternative. By combining a HILIC mobile phase, that is highly organic with a low water content, and an ion exchange column, a distinct layer system develops. When the analyte's charge is of the same direction as the stationary phase, retention and elution are determined by two antagonistic forces: electrostatic repulsion and hydrophilicity. One prominent group of challenging polar analytes are the polyamines cadaverine, putrescine, spermidine, and spermine. Carrying charges from +2 to +4 at physiological pH, these compounds are essential cell constituents and found in all living organisms. However, they are still notoriously challenging to analyze via the established liquid chromatography methods. In the present work, an ERLIC tandem mass spectrometry method has been exemplarily developed, optimized, and validated for the quantitative determination of cadaverine, putrescine, spermidine, and spermine. This method enables symmetrical peak shapes and good separation of analytes with different charges while simultaneously selectively detecting the co-eluting diamines by MS/MS. Furthermore, high linearity (R > 0.998) and sensitivity (LODs ≤ 2 ng/mL) have been proven. Thus, ERLIC may be interesting for both targeted and untargeted analysis approaches of highly charged low molecular weight organic molecules.


Assuntos
Poliaminas , Espectrometria de Massas em Tandem , Espectrometria de Massas em Tandem/métodos , Eletricidade Estática , Putrescina , Espermidina , Espermina , Cadaverina , Cromatografia Gasosa-Espectrometria de Massas , Cromatografia Líquida/métodos , Interações Hidrofóbicas e Hidrofílicas
16.
Artigo em Inglês | MEDLINE | ID: mdl-38547700

RESUMO

Glycopeptide enrichment is a crucial step in glycoproteomic analysis, often achieved through solid-phase extraction (SPE) on polar stationary phases in hydrophilic interaction liquid chromatography (HILIC). This study explores the potential of polyaniline (PANI)-coated silica gel for enriching human immunoglobulin G (IgG). Experimental conditions were varied to assess their impact on glycopeptide enrichment efficiency, comparing PANI-cotton wool SPE with conventional cotton wool as SPE sorbents. Two formic acid concentrations (0.1% and 1%) in elution solvent were tested, revealing that higher concentrations led to earlier elution of studied glycopeptides, especially for sialylated glycopeptides. Substituting formic acid with acetic acid increased the interaction of neutral glycopeptides with the PANI-modified sorbent, while sialylated glycopeptides showed no significant change in enrichment efficiency. Acetonitrile concentration in the elution solvent (5%, 10%, and 20%) affected the enrichment efficiency with most glycopeptides eluting at the lowest acetonitrile concentration. The acetonitrile concentration in conditioning and washing solutions (65%, 75%, and 85%) played a crucial role; at 65% acetonitrile, glycopeptides were least retained on the stationary phase, and neutral glycopeptides were even detected in the flow-through fraction. This study shows the potential of in-house-prepared PANI-modified sorbents for SPE-HILIC glycopeptide enrichment, highlighting the crucial role of tuning experimental conditions in sample preparation to enhance enrichment efficiency and selectivity.


Assuntos
Compostos de Anilina , Formiatos , Glicopeptídeos , Extração em Fase Sólida , Humanos , Glicopeptídeos/química , Cromatografia Líquida/métodos , Solventes , Extração em Fase Sólida/métodos , Interações Hidrofóbicas e Hidrofílicas , Acetonitrilas
17.
J Chromatogr A ; 1721: 464833, 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38555828

RESUMO

A 3 µm undecylenic acid-functionalized stationary phase (UAS) was prepared for the separation of nucleosides and nucleobases using per aqueous liquid chromatography (PALC) and hydrophilic interaction liquid chromatography (HILIC). The retention behaviors of nucleosides and nucleobases in PALC and HILIC modes were explored by adjusting parameters such as water content, buffer concentration, pH of the mobile phase and column temperature. The experimental data and separation chromatogram demonstrated that PALC could provide retention comparable to that of HILIC for nucleosides and nucleobases. Comparative studies using diluted adenosine solutions evaluated theoretical plates and peak shape for the same retention factors (between 0.25 and 5.0) in PALC and HILIC. There was no buffer component in the mobile phases used to operate the comparisons. HILIC mode is more efficient for adenosine than PALC mode at low retention factors. It's the exact opposite phenomenon for high retention factors. It is proposed that the mass transfer of adenosine between the UAS, the water-rich layer and the ACN-rich mobile phase in HILIC is relatively slow. Given the significant use of toxic ACN in HILIC, PALC emerges as a safer and more effective alternative for separating nucleosides and nucleobases.


Assuntos
Nucleosídeos , Dióxido de Silício , Ácidos Undecilênicos , Dióxido de Silício/química , Cromatografia Líquida/métodos , Interações Hidrofóbicas e Hidrofílicas , Água/química , Indicadores e Reagentes , Adenosina
18.
Adv Colloid Interface Sci ; 326: 103121, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38457900

RESUMO

Conventional drug delivery systems are associated with various shortcomings, including low bioavailability and limited control over release. Biodegradable polymeric microparticles have emerged as versatile carriers in drug delivery systems addressing all these challenges. This comprehensive review explores the dynamic landscape of microparticles, considering the role of hydrophilic and hydrophobic materials. Within the continuously evolving domain of microparticle preparation methods, this review offers valuable insights into the latest advancements and addresses the factors influencing microencapsulation, which is pivotal for harnessing the full potential of microparticles. Exploration of the latest research in this dynamic field unlocks the possibilities of optimizing microencapsulation techniques to produce microparticles of desired characteristics and properties for different applications, which can help contribute to the ongoing evolution in the field of pharmaceutical science.


Assuntos
Sistemas de Liberação de Medicamentos , Polímeros , Polímeros/química , Microesferas , Preparações Farmacêuticas , Interações Hidrofóbicas e Hidrofílicas
19.
Curr Protoc ; 4(3): e1013, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38483118

RESUMO

Universal solid supports are widely used in solid-phase oligonucleotide (ON) synthesis based on phosphoramidite chemistry. Herein, we describe the synthesis of hydrophobic universal linkers, namely phenanthrene ring-fused 7-oxabicyclo[2.2.1]heptane-2,3-diol derivatives (PT linkers), their coupling to solid supports [e.g., controlled pore glass (CPG) and polystyrene (PS)], and the use of the resulting PT-linker-modified solid supports in ON synthesis. PT linkers were synthesized in four steps from commercial materials and subsequently attached to CPG and PS resins through succinyl and diethylene glycol-containing spacers, respectively. Cleavage of the desired ON from the resins was accomplished under standard basic conditions, indicating that the reactivity of the PT linkers was comparable to that of conventional universal linkers. Furthermore, owing to their high hydrophobicity, the desired ON could be readily separated from impurities originating from the PT linker by reversed phase HPLC. © 2024 Wiley Periodicals LLC. Basic Protocol 1: Synthesis of phenanthrene ring-fused 7-oxabicyclo[2.2.1]heptane-2,3-diol (PT linker) derivatives Basic Protocol 2: Preparation of PT-linker-modified CPG and PS resins Basic Protocol 3: Solid-phase ON synthesis using PT-linker-modified solid supports and cleavage of ONs from resins.


Assuntos
Heptanos , Oligonucleotídeos , Oligonucleotídeos/química , Interações Hidrofóbicas e Hidrofílicas
20.
Carbohydr Polym ; 333: 121981, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38494233

RESUMO

In view of health and environmental concerns, together with the upcoming restrictive regulations on per- and polyfluoroalkyl substances (PFAS), less impactful materials must be explored for the hydrophobization of surfaces. Polysaccharides, and especially chitosan, are being explored for their desirable properties of film formation and ease of modification. We present a PFAS-free chitosan superhydrophobic coating for textiles deposited through a solvent-free method. By contact angle analysis and drop impact, we observe that the coating imparts hydrophobicity to the fabrics, reaching superhydrophobicty (θA = 151°, θR = 136°) with increased amount of coating (from 1.6 g/cm2). This effect is obtained by the combination of chemical water repellency of the modified chitosan and the nano- and micro-roughness, assessed by SEM analysis. We perform a comprehensive study on the durability of the coatings, showing good results especially for acidic soaking where the hydrophobicity is maintained until the 8th cycle of washing. We assess the degradation of the coating by a TGA-IR investigation to define the compounds released with thermal degradation, and we confirm the coating's biodegradability by biochemical oxygen consumption. Finally, we demonstrate its biocompatibility on keratinocytes (HaCaT cell line) and fibroblasts (HFF-1 cell line), confirming that the coating is safe for human skin cells.


Assuntos
Quitosana , Humanos , Interações Hidrofóbicas e Hidrofílicas , Solventes , Fibroblastos , Ácidos
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