Morphology and Rheology of a Cool-Gel (Protein) Blended with a Thermo-Gel (Hydroxypropyl Methylcellulose).
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ABSTRACT:
SUBMITTER: Ji Z
PROVIDER: S-EPMC8750888 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Sol-gel transformations in HPMC (hydroxypropyl methylcellulose) are being increasingly studied because of their role in bio-related applications. The thermo-reversible behavior of HPMC is particularly affected by its properties and concentration in solvent media, nature of additives, and the thermal environment it is exposed to. This article contains investigations on the effects of salt additives in Hofmeister series on the HPMC gelation. Various findings regarding gelation with salt ions as well as with the ionic and non-ionic surfactants are presented. The gel formation in physiological salt fluids such as simulated gastric and intestine fluids is also examined with the interest in oral drug delivery systems. The processes of swelling, dissolution and dispersion of HPMC tablets in simulated bio-fluids are explored and the release of a drug from the tablet affected by such processes is studied. Explanations are provided based on the chemical structure and the molecular binding/association of HPMC in a media. The test results at the body or near-body temperature conditions helped in understanding the progress of the gelation process within the human body environment. The detailed interpretation of various molecule level interactions unfolded the sol-gel mechanisms and the influence of a few other factors. The obtained test data and the established mathematical models are expected to serve as a guide in customizing applications of HPMC hydrogels.
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Project description:Diet influences host metabolism and intestinal microbiota; however, detailed understanding of this tripartite interaction is limited. To determine whether the nonfermentable fiber hydroxypropyl methylcellulose (HPMC) could alter the intestinal microbiota and whether such changes correlated with metabolic improvements, C57B/L6 mice were normalized to a high-fat diet (HFD), then either maintained on HFD (control), or switched to HFD supplemented with 10% HPMC, or a low-fat diet (LFD). Compared to control treatment, both LFD and HPMC reduced weight gain (11.8 and 5.7 g, respectively), plasma cholesterol (23.1 and 19.6%), and liver triglycerides (73.1 and 44.6%), and, as revealed by 454-pyrosequencing of the microbial 16S rRNA gene, decreased microbial ?-diversity and differentially altered intestinal microbiota. Both LFD and HPMC increased intestinal Erysipelotrichaceae (7.3- and 12.4-fold) and decreased Lachnospiraceae (2.0- and 2.7-fold), while only HPMC increased Peptostreptococcaceae (3.4-fold) and decreased Ruminococcaceae (2.7-fold). Specific microorganisms were directly linked with weight change and metabolic parameters in HPMC and HFD mice, but not in LFD mice, indicating that the intestinal microbiota may play differing roles during the two dietary modulations. This work indicates that HPMC is a potential prebiotic fiber that influences intestinal microbiota and improves host metabolism.
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Project description:The present study aims to investigate the degradation of HPMC on a laboratory scale by acoustic and hydrodynamic cavitation. The effects of temperature and the addition of an external oxidizing agent on the effectiveness of HPMC degradation were systematically investigated by SEC/MALS-RI, FTIR and 1H NMR. The results of the experiments without cavitation show that an external oxidizing agent alone reduces the weight-average molar mass at 60 °C in 30 min for 45.1 % (from 335 to 184 kg mol-1). However, the weight-average molar mass of HPMC decreased significantly more in the cavitation treatment, for 98.8 % (from 335 to 4 kg mol-1) in 30 min at optimal operating conditions of hydrodynamic cavitation (i.e. addition of external oxidant and 60 °C) with a concomitant narrowing of the molar mass distribution, as shown by the dispersity value, which decreased from 2.24 to 1.31. Compared to acoustic cavitation, hydrodynamic cavitation also proved to be more energy efficient. The FTIR spectra of the cavitated HPMC samples without the addition of H2O2 show negligible oxidation of the hydroxyl groups and the glycosidic bonds, confirming that mechanical effects predominate in HPMC degradation in these cases. In contrast, when H2O2 was added, FTIR and 1H NMR show typical signals for cellulose oxidation products, especially when the experiments were performed at 60 °C, confirming that chemical as well as mechanical effects are responsible for the extensive HPMC degradation in these cases. Since treatment methods that lead to lower molar masses and narrower molar mass distributions of the polymers are lacking or require longer treatment times (e.g. 24 h), mechanochemical treatment methods such as cavitation have great potential, as they enable faster polymer degradation (in our case 30 min) through a combination of mechanical and/or chemical degradation mechanisms.
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Project description:Three-dimensional (3D) bioprinting has emerged as an important tool to fabricate scaffolds with complex structures for tissue engineering and regenerative medicine applications. For extrusion-based 3D bioprinting, the success of printing complex structures relies largely on the properties of bioink. Methylcellulose (MC) has been exploited as a potential bioink for 3D bioprinting due to its temperature-dependent rheological properties. However, MC is highly soluble and has low structural stability at room temperature, making it suboptimal for 3D bioprinting applications. In this study, we report a one-step synthesis protocol for modifying MC with norbornene (MCNB), which serves as a new bioink for 3D bioprinting. MCNB preserves the temperature-dependent reversible sol-gel transition and readily reacts with thiol-bearing linkers through light-mediated step-growth thiol-norbornene photopolymerization. Furthermore, we rendered the otherwise inert MC network bioactive through facile conjugation of integrin-binding ligands (e.g. CRGDS) or via incorporating cell-adhesive and protease-sensitive gelatin-based macromer (e.g. GelNB). The adaptability of the new MCNB-based bioink offers an attractive option for diverse 3D bioprinting applications.
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Project description:The purpose of this work was to develop a simple method to produce self-supported films composed of hydroxypropyl methylcellulose (HPMC) and polyaniline (PANI) by the direct mixture of aqueous dispersions of both polymers with subsequent drying. The addition of HPMC, a cellulose derivative with an excellent film-forming capacity, was fundamental to overcoming the poor processability of PANI, which impairs its use in many technological applications. All films showed conductivity in the order of 10-2 to 10-3 S cm-1, which is in the range for metals or semiconductors. The typical electroactivity of PANI was also maintained in the hybrid films. The thermal stability and the mechanical properties of the pristine PANI were also improved with the addition of HPMC. Cellulose-containing conducting polymers can be considered a material of the future, with possible applications in several areas, such as smart wallpapers, e-papers, and sensors.
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Project description:Tissue-specific patterned stem cell differentiation serves as the basis for the development, remodeling, and regeneration of the multicellular structure of the native tissues. We herein proposed a cytocompatible 3D casting process to recapitulate this patterned stem cell differentiation for reconstructing multicellular tissues in vitro. We first reconstituted the 2D culture conditions for stem cell fate control within 3D hydrogel by incorporating the sets of the diffusible signal molecules delivered through drug-releasing microparticles. Then, utilizing thermo-responsivity of methylcellulose (MC), we developed a cytocompatible casting process to mold these hydrogels into specific 3D configurations, generating the targeted spatial gradients of diffusible signal molecules. The liquid phase of the MC solution was viscous enough to adopt the shapes of 3D impression patterns, while the gelated MC served as a reliable mold for patterning the hydrogel prepolymers. When these patterned hydrogels were integrated together, the stem cells in each hydrogel distinctly differentiated toward individually defined fates, resulting in the formation of the multicellular tissue structure bearing the very structural integrity and characteristics as seen in vascularized bones and osteochondral tissues.
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Project description:The ongoing coronavirus disease (COVID-19) pandemic has required a variety of non-medical interventions to limit the transmission of the causative agent, severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). One such option is over-the-counter nasal sprays that aim to block virus entry and transmission within the nasal cavity. In this study, we assessed the ability of three hydroxypropyl methylcellulose (HPMC)-based powder nasal sprays, produced by Nasaleze, to inhibit SARS-CoV-2 infection and release in vitro. Upon application, the HPMC powder forms a gel-like matrix within the nasal cavity-a process we recapitulated in cell culture. We found that virus release from cells previously infected with SARS-CoV-2 was inhibited by the gel matrix product in a dose-dependent manner, with virus levels reduced by >99.99% over a 72 h period at a dose of 6.4 mg/3.5 cm2. We also show that the pre-treatment of cells with product inhibited SARS-CoV-2 infection, independent of the virus variant. The primary mechanism of action appears to be via the formation of a physical, passive barrier. However, the addition of wild garlic provided additional direct antiviral properties in some formulations. We conclude that HPMC-based nasal sprays may offer an additional component to strategies to limit the spread of respiratory viruses, including SARS-CoV-2.
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Project description:The mechanical and thermal properties of cryogels depend on their microstructure. In this study, the microstructure of hydroxypropyl methylcellulose (HPMC) cryogels was modified by the addition of ionic (bis (2-ethylhexyl) sodium sulfosuccinate, AOT) and non-ionic (Kolliphor® EL) surfactants to the precursor hydrogels (30 g/L). The surfactant concentrations varied from 0.2 mmol/L to 3.0 mmol/L. All of the hydrogels presented viscous behavior (G″ > G'). Hydrogels containing AOT (c > 2.0 mmol/L) led to cryogels with the lowest compressive modulus (13 ± 1 kPa), the highest specific surface area (2.31 m2/g), the lowest thermal conductivity (0.030 W/(m·°C)), and less hygroscopic walls. The addition of Kolliphor® EL to the hydrogels yielded the stiffest cryogels (320 ± 32 kPa) with the lowest specific surface area (1.11 m2/g) and the highest thermal conductivity (0.055 W/(m·°C)). Density functional theory (DFT) calculations indicated an interaction energy of -31.8 kcal/mol due to the interaction between the AOT sulfonate group and the HPMC hydroxyl group and the hydrogen bond between the AOT carbonyl group and the HPMC hydroxyl group. The interaction energy between the HPMC hydroxyl group and the Kolliphor® EL hydroxyl group was calculated as -7.91 kcal/mol. A model was proposed to describe the effects of AOT or Kolliphor® EL on the microstructures and the mechanical/thermal properties of HPMC cryogels.
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Project description:Hydroxypropyl cellulose (HPC) is a surface active polymer that can change its solubility as a function of temperature. This makes HPC interesting for responsive foams, where macroscopic properties need to be reversibly changed on demand. Analysis of aqueous HPC foams as a function of temperature showed a moderate decrease in foam half-life time from 9000 to 4000 s, when the temperature was increased. However, within a narrow temperature range of ±2 °C a dramatic decrease in half-life time to <120 s was observed at 43 °C in the absence and at 31 °C in the presence of 0.7 M NaCl. These drastic changes are highly reversible and are associated to the lower critical solution temperatures (LCST) of HPC in aqueous solutions. In fact, dynamic light scattering experiments indicate that HPC molecules form aggregates at temperatures >31 °C (0.7 M NaCl) and >43 °C (0 M NaCl), which shrink in size when the temperature is increased further. From these results, we conclude that the LCST of 1 MDa HPC is at 43 °C when no salt is present and is at 31 °C in aqueous solutions with 0.7 M NaCl. In addition, shear rheology of bulk solutions and surface tensiometry indicate that the solution's viscosity and the surface pressure dramatically change at the respective LCSTs. Obviously, the solvent's viscosity triggers substantial changes in foam drainage at the LCST, which is shown to be the main driving force for the temperature responsiveness of HPC foams.
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Project description:Changes in tensile properties and the glass transition temperature (Tg) of plasticized polymer films are typically attributed to molecular mobility, often with no empirical data to support such an assertion. Herein solvent cast HPMC films containing varying amounts of PEG, as the plasticizer, were used to assess the dependence of tensile properties and the Tg on glassy state molecular mobility. Molecular mobility (molecular relaxation time and temperature) parameters were determined by Thermally Stimulated Current Spectroscopy (TSC). The tensile properties and Tg of the HPMC films were determined by texture analysis and DSC, respectively. Molecular mobilities detected by TSC were cooperative and occurred at temperatures (Tg') well below (113 to 127?°C) the bulk Tg. The relaxation times (?) were 71?±?1, 46?±?1, 42?±?1, 36?±?1 and 29?±?1?s for HPMC films containing 0, 6, 8, 11 and 17% (w/w) PEG, respectively. The Tg and glassy state molecular mobility were found to be intimately linked and demonstrated a linear dependence. While tensile strength was found to be linearly related to molecular relaxation time, tensile elongation and elastic modulus exhibited a non-linear dependence on molecular mobility. The data presented in this work demonstrates the complex nature of the relationship between plasticizer content, molecular mobility, Tg and tensile properties for plasticized polymeric films. It highlights the fact that the dependence of the bulk physico-mechanical properties on glassy state molecular mobility, differ greatly. Therefore, empirical characterization of molecular mobility is important to fully understand and predict the thermo-mechanical behavior of plasticized polymer films. This work demonstrates the unique capability of TSC to provide key information relating to molecular mobility and its influence on the bulk properties of materials. Data generated using TSC could prove useful for stability and performance ranking, in addition to the ability to predict materials behavior using data generated at or below typical storage conditions in the pharmaceutical, food, and polymer industries.
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