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1.
AAPS PharmSciTech ; 25(6): 156, 2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38981986

ABSTRACT

Commercial topical formulations containing itraconazole (poorly water soluble), for mycotic infections, have poor penetration to infection sites beneath the nails and skin thereby necessitating oral administration. To improve penetration, colloidal solutions of itraconazole (G1-G4) containing Poloxamer 188, tween 80, ethanol, and propylene glycol were prepared and incorporated into HFA-134-containing sprays. Formulations were characterized using particle size, drug content, and Fourier-transform infrared spectroscopy (FTIR). In vitro permeation studies were performed using Franz diffusion cells for 8 h. Antimycotic activity on Candida albicans and Trichophyton rubrum was performed using broth micro-dilution and flow cytometry, while cytotoxicity was tested on HaCaT cell lines. Particle size ranged from 39.35-116.80 nm. FTIR and drug content revealed that G1 was the most stable formulation (optimized formulation). In vitro release over 2 h was 45% for G1 and 34% for the cream. There was a twofold increase in skin permeation, fivefold intradermal retention, and a sevenfold increase in nail penetration of G1 over the cream. Minimum fungicidal concentrations (MFC) against C. albicans were 0.156 and 0.313 µg/mL for G1 and cream, respectively. The formulations showed optimum killing kinetics after 48 h. MFC values against T. rubrum were 0.312 and 0.625 µg/mL for the G1 and cream, respectively. Transmission electron microscopy revealed organelle destruction and cell leakage for G1 in both organisms and penetration of keratin layers to destroy T. rubrum. Cytotoxicity evaluation of G1 showed relative safety for skin cells. The G1 formulation showed superior skin permeation, nail penetration, and fungicidal activity compared with the cream formulation.


Subject(s)
Antifungal Agents , Candida albicans , Colloids , Itraconazole , Antifungal Agents/pharmacology , Antifungal Agents/administration & dosage , Candida albicans/drug effects , Itraconazole/pharmacology , Itraconazole/administration & dosage , Itraconazole/chemistry , Humans , Animals , Trichophyton/drug effects , Microbial Sensitivity Tests/methods , Chemistry, Pharmaceutical/methods , Particle Size , Skin/metabolism , Skin/drug effects , Skin/microbiology , Skin Absorption/drug effects , Cell Line , HaCaT Cells , Nails/drug effects , Nails/microbiology , Nails/metabolism , Arthrodermataceae
2.
J Med Chem ; 67(12): 10263-10274, 2024 Jun 27.
Article in English | MEDLINE | ID: mdl-38864383

ABSTRACT

Colloidal aggregation is one of the largest contributors to false positives in early drug discovery. Here, we consider aggregation's role in cell-based infectivity assays in Covid-19 drug repurposing. We investigated the potential aggregation of 41 drug candidates reported as SARs-CoV-2 entry inhibitors. Of these, 17 formed colloidal particles by dynamic light scattering and exhibited detergent-dependent enzyme inhibition. To evaluate the impact of aggregation on antiviral efficacy in cells, we presaturated the colloidal drug suspensions with BSA or spun them down by centrifugation and measured the effects on spike pseudovirus infectivity. Antiviral potencies diminished by at least 10-fold following both BSA and centrifugation treatments, supporting a colloid-based mechanism. Aggregates induced puncta of the labeled spike protein in fluorescence microscopy, consistent with sequestration of the protein on the colloidal particles. These observations suggest that colloidal aggregation is common among cell-based antiviral drug repurposing and offers rapid counter-screens to detect and eliminate these artifacts.


Subject(s)
Antiviral Agents , Colloids , SARS-CoV-2 , Antiviral Agents/pharmacology , Antiviral Agents/chemistry , Humans , SARS-CoV-2/drug effects , Colloids/chemistry , Spike Glycoprotein, Coronavirus/metabolism , COVID-19 Drug Treatment , Drug Repositioning , COVID-19/virology
3.
J Food Sci ; 89(7): 4359-4371, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38847748

ABSTRACT

Hydrocolloids are widely used in meat products as common food additives. However, research has indicated that excessive consumption of these hydrocolloids may have potential health implications. Currently, consumers mainly rely on sensory evaluation to identify hydrocolloid adulteration in meat products. Although many studies on quantitative detection of hydrocolloids have been conducted by biochemical methods in laboratory environments, there is currently a lack of effective tools for consumers and regulators to obtain real-time and reliable information on hydrocolloid adulteration. To address this challenge, a smartphone-based computer vision method was developed to quantitatively detect carrageenan adulteration in beef in this work. Specifically, Swin Transformer models, along with pre-training and fine-tuning techniques, were used to successfully automate the classification of beef into nine different levels of carrageenan adulteration, ranging from 0% to 20%. Among the tested models, Swin-Tiny (Swin-T) achieved the highest trade-off performance, with a Top-1 accuracy of 0.997, a detection speed of 3.2 ms, and a model size of 103.45 Mb. Compared to computer vision, the electrochemical impedance spectroscopy achieved a lower accuracy of 0.792 and required a constant temperature environment and a waiting time of around 30 min for data stabilization. In addition, Swin-T model was also capable of distinguishing between different types of hydrocolloids with a Top-1 accuracy of 0.975. This study provides consumers and regulators with a valuable tool to obtain real-time quantitative information about meat adulteration anytime, anywhere. PRACTICAL APPLICATION: This research provides a practical solution for regulators and consumers to non-destructively and quantitatively detect the content and type of hydrocolloids in beef in real-time using smartphones. This innovation has the potential to significantly reduce the costs associated with meat quality testing, such as the use of chemical reagents and expensive instruments.


Subject(s)
Carrageenan , Colloids , Food Contamination , Smartphone , Food Contamination/analysis , Colloids/chemistry , Animals , Cattle , Carrageenan/analysis , Carrageenan/chemistry , Meat Products/analysis , Food Additives/analysis , Red Meat/analysis , Meat/analysis
4.
Environ Sci Technol ; 58(27): 12113-12122, 2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38917351

ABSTRACT

Size and purity of metal phosphate and metal sulfide colloids can control the solubility, persistence, and bioavailability of metals in environmental systems. Despite their importance, methods for detecting and characterizing the diversity in the elemental composition of these colloids in complex matrices are missing. Here, we develop a single-particle inductively coupled plasma time-of-flight mass spectrometry (sp-icpTOF-MS) approach to characterize the elemental compositions of individual metal phosphate and sulfide colloids extracted from complex matrices. The stoichiometry was accurately determined for particles of known composition with an equivalent spherical diameter of ≥∼200 nm. Assisted by machine learning (ML), the new method could distinguish particles of the copper sulfides covellite (CuS), chalcocite (Cu2S), and chalcopyrite particles (CuFeS2) with 75% (for Cu2S) to 99% (for CuFeS2) accuracy. Application of the sp-icpTOF-MS method to particles recovered from natural samples revealed that iron sulfide (FeS) particles in lake sediment contained ∼4% copper and zinc impurities, whereas pure pyrite (FeS2) was identified in hydraulic fracturing wastewater and confirmed by selected area electron diffraction. Colloidal mercury in an offshore marine sediment was present as pure mercury sulfide (HgS), whereas geogenic HgS recovered from an industrial process contained ∼0.08 wt % silver per Hg, enabling source apportionment of these colloids using ML. X-ray absorption spectroscopy confirmed that Hg was predominantly present as metacinnabar (ß-HgS) in the industrial process sample. The determination of impurities in individual colloids, such as zinc and copper in FeS, and silver in HgS may enable improved assessment of their origin, reactivity, and bioavailability potential.


Subject(s)
Colloids , Mass Spectrometry , Phosphates , Soil , Sulfides , Colloids/chemistry , Sulfides/chemistry , Soil/chemistry , Phosphates/chemistry , Geologic Sediments/chemistry , Metals/chemistry
5.
J Chem Inf Model ; 64(13): 4991-5005, 2024 Jul 08.
Article in English | MEDLINE | ID: mdl-38920403

ABSTRACT

The ability to conduct effective high throughput screening (HTS) campaigns in drug discovery is often hampered by the detection of false positives in these assays due to small colloidally aggregating molecules (SCAMs). SCAMs can produce artifactual hits in HTS by nonspecific inhibition of the protein target. In this work, we present a new computational prediction tool for detecting SCAMs based on their 2D chemical structure. The tool, called the boosted aggregation detection (BAD) molecule filter, employs decision tree ensemble methods, namely, the CatBoost classifier and the light gradient-boosting machine, to significantly improve the detection of SCAMs. In developing the filter, we explore models trained on individual data sets, a consensus approach using these models, and, third, a merged data set approach, each tailored for specific drug discovery needs. The individual data set method emerged as most effective, achieving 93% sensitivity and 90% specificity, outperforming existing state-of-the-art models by 20 and 5%, respectively. The consensus models offer broader chemical space coverage, exceeding 90% for all testing sets. This feature is an important aspect particularly for early stage medicinal chemistry projects, and provides information on applicability domain. Meanwhile, the merged data set models demonstrated robust performance, with a notable sensitivity of 79% in the comprehensive 10-fold cross-validation test set. A SHAP analysis of model features indicates the importance of hydrophobicity and molecular complexity as primary factors influencing the aggregation propensity. The BAD molecule filter is readily accessible for the public usage on https://molmodlab-aau.com/Tools.html. This filter provides a new, more robust tool for aggregate prediction in the early stages of drug discovery to optimize hit rates and reduce associated testing and validation overheads.


Subject(s)
Drug Discovery , Drug Discovery/methods , Colloids/chemistry , High-Throughput Screening Assays , Small Molecule Libraries/chemistry
6.
Int J Biol Macromol ; 272(Pt 2): 132773, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38823746

ABSTRACT

The structure and physicochemical properties of the complex system of peanut protein and gluten with different concentrations (0 %, 0.5 %, 1 %, and 2 %) of carboxymethyl cellulose (CMC) or sodium alginate (SA) under high-moisture extrusion were studied. The water absorption index and low-field nuclear magnetic resonance showed that adding 0.5 % SA could significantly improve the water uniformity of peanut protein extrudates, while the increase in water absorption was not significant. The texture properties showed that adding CMC or SA increased the hardness, vertical shearing force, and parallel shearing force of the system. Furthermore, adding 0.5 % SA increased approximately 33 % and 75.2 % of the tensile distance and strength of the system, respectively. The secondary structure showed that CMC or SA decreased the proportion of α-helix, ß-turn, and random coil, while increased ß-sheet proportion. The results of hydrophobicity, unextractable protein, and endogenous fluorescence revealed that CMC and SA reduced the surface hydrophobicity of the system and caused fluorescence quenching in the system. Additionally, it was found that CMC generally increased the free sulfhydryl group content, while SA exhibited the opposite effect.


Subject(s)
Arachis , Colloids , Glutens , Plant Proteins , Polysaccharides , Triticum , Glutens/chemistry , Arachis/chemistry , Colloids/chemistry , Plant Proteins/chemistry , Polysaccharides/chemistry , Polysaccharides/pharmacology , Triticum/chemistry , Chemical Phenomena , Water/chemistry , Hydrophobic and Hydrophilic Interactions , Carboxymethylcellulose Sodium/chemistry , Tensile Strength , Alginates/chemistry , Alginates/pharmacology
7.
Langmuir ; 40(23): 11936-11946, 2024 Jun 11.
Article in English | MEDLINE | ID: mdl-38797979

ABSTRACT

Lipid/copolymer colloidal systems are deemed hybrid materials with unique properties and functionalities. Their hybrid nature leads to complex interfacial phenomena, which have not been fully encoded yet, navigating their properties. Moving toward in-depth knowledge of such systems, a comprehensive investigation of them is imperative. In the present study, hybrid lipid/copolymer structures were fabricated and examined by a gamut of techniques, including dynamic light scattering, fluorescence spectroscopy, cryogenic transmission electron microscopy, microcalorimetry, and high-resolution ultrasound spectroscopy. The biomaterials that were mixed for this purpose at different ratios were 1,2-dioctadecanoyl-sn-glycero-3-phosphocholine and four different linear, statistical (random) amphiphilic copolymers, consisting of oligo(ethylene glycol) methyl ether methacrylate as the hydrophilic comonomer and lauryl methacrylate as the hydrophobic one. The colloidal dispersions were studied for lipid/copolymer interactions regarding their physicochemical, morphological, and biophysical behavior. Their membrane properties and interactions with serum proteins were also studied. The aforementioned techniques confirmed the hybrid nature of the systems and the location of the copolymer in the structure. More importantly, the random architecture of the copolymers, the hydrophobic-to-hydrophilic balance of the nanoplatforms, and the lipid-to-polymer ratio are highlighted as the main design-influencing factors. Elucidating the lipid/copolymer interactions would contribute to the translation of hybrid nanoparticle performance and, thus, their rational design for multiple applications, including drug delivery.


Subject(s)
Colloids , Colloids/chemistry , Polymers/chemistry , Hydrophobic and Hydrophilic Interactions , Polyethylene Glycols/chemistry , Methacrylates/chemistry
8.
Nature ; 630(8017): 648-653, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38811735

ABSTRACT

Colloidal crystals exhibit interesting properties1-4 that are in many ways analogous to their atomic counterparts. They have the same crystal structures2,5-7, undergo the same phase transitions8-10, and possess the same crystallographic defects11-14. In contrast to these structural properties, the mechanical properties of colloidal crystals are quite different from those of atomic systems. For example, unlike in atomic systems, the elasticity of hard-sphere colloidal crystals is purely entropic15; as a result, they are so soft that they can be melted just by stirring16,17. Moreover, crystalline materials deform plastically when subjected to increasing shear and become stronger because of the ubiquitous process of work hardening18; but this has so far never been observed in colloidal crystals, to our knowledge. Here we show that hard-sphere colloidal crystals exhibit work hardening. Moreover, despite their softness, the shear strength of colloidal crystals can increase and approach the theoretical limit for crystals, a value reached in very few other materials so far. We use confocal microscopy to show that the strength of colloidal crystals increases with dislocation density, and ultimately reaches the classic Taylor scaling behaviour for atomic materials19-21, although hard-sphere interactions lack the complexity of atomic interactions. We demonstrate that Taylor hardening arises through the formation of dislocation junctions22. The Taylor hardening regime, however, is established only after a transient phase, and it ceases when the colloidal crystals become so hard that the strain is localized within a thin boundary layer in which slip results from an unconventional motion of dislocations. The striking resemblance between colloidal and atomic crystals, despite the many orders of magnitude difference in particle size and shear modulus, demonstrates the universality of work hardening.


Subject(s)
Colloids , Crystallization , Colloids/chemistry , Microscopy, Confocal , Shear Strength , Hardness , Elasticity
9.
Food Chem ; 454: 139650, 2024 Oct 01.
Article in English | MEDLINE | ID: mdl-38788478

ABSTRACT

Inspired by the desert beetle, a novel biomimetic chip was developed to detect chloramphenicol (CP). The chip was characterized by a periodic array in which hydrophobic Au nanoparticles (AuNPs) were semi-embedded on hydrophilic polymethyl methacrylate (PMMA) spheres. Among them, the AuNPs exhibited both a localized surface plasmon resonance effect to amplify the reflected signal and a synergistic effect with PMMA spheres to create a significant hydrophilic-hydrophobic interface, which facilitated the enrichment of target CP molecules and improved sensitivity. After optimization, the chip showed direct, ultrasensitive (as low as 0.2 ng/mL), fast (5 min), and selective detection of CP with a wide concentration range extending from 0.2 ng/mL to 1000 ng/mL. During detection, color changes of the chip were observed by naked eyes without any color display equipment. The recovery of CP was between 94.65 % and 108.70 % in chicken and milk samples.


Subject(s)
Chickens , Chloramphenicol , Coleoptera , Food Contamination , Gold , Metal Nanoparticles , Milk , Chloramphenicol/analysis , Chloramphenicol/chemistry , Animals , Gold/chemistry , Metal Nanoparticles/chemistry , Coleoptera/chemistry , Food Contamination/analysis , Milk/chemistry , Anti-Bacterial Agents/analysis , Anti-Bacterial Agents/chemistry , Colloids/chemistry
10.
Biomacromolecules ; 25(6): 3703-3714, 2024 Jun 10.
Article in English | MEDLINE | ID: mdl-38806282

ABSTRACT

As a versatile nanomaterial derived from renewable sources, nanocellulose has attracted considerable attention for its potential applications in various sectors, especially those focused on water treatment and remediation. Here, we have combined atomic force microscopy (AFM) and reactive molecular dynamics (RMD) simulations to characterize the interactions between cellulose nanofibers modified with carboxylate or phosphate groups and the protein foulant model bovine serum albumin (BSA) at pH 3.92, which is close to the isoelectric point of BSA. Colloidal probes were prepared by modification of the AFM probes with the nanofibers, and the nanofiber coating on the AFM tip was for the first time confirmed through fluorescence labeling and confocal optical sectioning. We have found that the wet-state normalized adhesion force is approximately 17.87 ± 8.58 pN/nm for the carboxylated cellulose nanofibers (TOCNF) and about 11.70 ± 2.97 pN/nm for the phosphorylated ones (PCNF) at the studied pH. Moreover, the adsorbed protein partially unfolded at the cellulose interface due to the secondary structure's loss of intramolecular hydrogen bonds. We demonstrate that nanocellulose colloidal probes can be used as a sensitive tool to reveal interactions with BSA at nano and molecular scales and under in situ conditions. RMD simulations helped to gain a molecular- and atomistic-level understanding of the differences between these findings. In the case of PCNF, partially solvated metal ions, preferentially bound to the phosphates, reduced the direct protein-cellulose connections. This understanding can lead to significant advancements in the development of cellulose-based antifouling surfaces and provide crucial insights for expanding the pH range of use and suggesting appropriate recalibrations.


Subject(s)
Cellulose , Microscopy, Atomic Force , Molecular Dynamics Simulation , Nanofibers , Serum Albumin, Bovine , Serum Albumin, Bovine/chemistry , Cellulose/chemistry , Nanofibers/chemistry , Animals , Cattle , Microscopy, Atomic Force/methods , Water/chemistry , Hydrogen Bonding , Colloids/chemistry , Hydrogen-Ion Concentration , Adsorption
11.
Colloids Surf B Biointerfaces ; 240: 113997, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38815309

ABSTRACT

In this paper, a simple, bottom up, bioinspired technique is proposed for the synthesis of highly stable colloids of silica supported spherical silver nanoparticles (SiO2@Ag) that act as efficient catalytic and antimicrobial coatings for an organic substrate, filter paper. The core - shell structure and the highly branched dendritic polymer, poly(ethylene)imine, enabled the precise control of growth rate and morphology of silica and silver nanoparticles. The polymer also enabled the deposition of these nanoparticles onto an organic substrate, filter paper, through immersion by modifying its surface. The catalytic and antibacterial properties of these samples were assessed. The results obtained from this analysis showed a complete degradation of an aqueous pollutant, 4-nitrophenol, for 6 successive catalytic cycles without intermediate purification steps. Furthermore, the polymeric silica-silver suspension proved to express antibacterial activity against both Gram-positive and Gram-negative bacteria (Escherichia coli, Staphylococcus aureus, Pseudomonas aeruginosa). The antibacterial properties were evaluated according to the disk diffusion method, whereas the Minimum Inhibitory Concentration was also determined. The samples were examined by Scanning Electron Microscopy, Transmission Electron Microscopy, X-ray diffraction analysis, z-potential analysis, Fourier Transform Infrared Spectroscopy and Ultraviolet-visible Spectroscopy.


Subject(s)
Anti-Bacterial Agents , Colloids , Microbial Sensitivity Tests , Silicon Dioxide , Silver , Silver/chemistry , Silver/pharmacology , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/chemical synthesis , Silicon Dioxide/chemistry , Silicon Dioxide/pharmacology , Catalysis , Colloids/chemistry , Metal Nanoparticles/chemistry , Polymers/chemistry , Polymers/pharmacology , Polymers/chemical synthesis , Escherichia coli/drug effects , Escherichia coli/growth & development , Paper , Staphylococcus aureus/drug effects , Pseudomonas aeruginosa/drug effects , Surface Properties , Particle Size , Nitrophenols/chemistry
12.
Food Chem ; 451: 139469, 2024 Sep 01.
Article in English | MEDLINE | ID: mdl-38703727

ABSTRACT

Excipient selection is crucial to address the oxidation and solubility challenges of bioactive substances, impacting their safety and efficacy. AKPL, a novel ω-3 polyunsaturated fatty acids (PUFAs) esterified phospholipid derived from Antarctic krill, demonstrates unique antioxidant capabilities and synergistic effects. It exhibits pronounced surface activity and electronegativity at physiological pH, as evidenced by a critical micelle concentration (CMC) of 0.15 g/L and ζ-potential of -49.9 mV. In aqueous environments, AKPL self-assembles into liposomal structures, offering high biocompatibility and promoting cell proliferation. Its polyunsaturated bond-rich structure provides additional oxidation sites, imparting antioxidant properties superior to other phospholipids like DSPC and DOPC. Additionally, AKPL augments the efficacy of lipophilic antioxidants, such as alpha-tocopherol and curcumin, in aqueous media through both intermolecular and intramolecular interactions. In sum, AKPL emerges as an innovative unsaturated phospholipid, offering new strategies for encapsulating and delivering oxygen-sensitive agents.


Subject(s)
Antioxidants , Euphausiacea , Phospholipids , Euphausiacea/chemistry , Animals , Phospholipids/chemistry , Antioxidants/chemistry , Antioxidants/pharmacology , Colloids/chemistry , Humans , Biocompatible Materials/chemistry , Biocompatible Materials/pharmacology , Antarctic Regions , Fatty Acids, Omega-3/chemistry , Fatty Acids, Omega-3/pharmacology
13.
Food Chem ; 452: 139474, 2024 Sep 15.
Article in English | MEDLINE | ID: mdl-38744126

ABSTRACT

In order to prevent the photooxidation of phytosterols, a new type of Pickering emulsion was developed by regulating the oriented distribution of antioxidants in colloidal lipid particles (CLPs) at the oil-water interface. High-melting-point and low-melting-point lipids were tested to modulate their protective effect against phytosterols photooxidation. Results showed that CLPs could stabilize Pickering emulsion and encapsulate antioxidants, providing a dual functional delivery system for phytosterols protection. The Pickering emulsion formed had a particle size of around 350-820 nm, and the crystallization and melting temperatures of tripalmitin particles were approximately 32 °C and 63.8 °C, respectively. The addition of tributyrin or tricaprylin reduced the crystallization and melting temperatures of Pal CLPs and improved the photooxidation emulsion stability. The prepared Pickering emulsion remained stable for a maximum of 12 days under accelerated light-induced oxidation. Among all formulations, the emulsion primarily composed of tripalmitin CLPs, with added tributyrin and resveratrol, exhibited the highest photooxidation stability.


Subject(s)
Antioxidants , Emulsions , Lipids , Oxidation-Reduction , Particle Size , Phytosterols , Emulsions/chemistry , Phytosterols/chemistry , Antioxidants/chemistry , Lipids/chemistry , Colloids/chemistry , Light , Drug Compounding , Drug Stability
14.
Int J Pharm ; 658: 124231, 2024 Jun 10.
Article in English | MEDLINE | ID: mdl-38759741

ABSTRACT

Two frequent problems hindering clinical translation of nanomedicine are low drug loading and low colloidal stability. Previous efforts to achieve ultrahigh drug loading (>30 %) introduce new hurdles, including lower colloidal stability and others, for clinical translation. Herein, we report a new class of drug nano-carriers based on our recent finding in protein-nanoparticle co-assembly supraparticle (PNCAS), with both ultrahigh drug loading (58 % for doxorubicin, i.e., DOX) and ultrahigh colloidal stability (no significant change in hydrodynamic size after one year). We further show that our PNCAS-based drug nano-carrier possesses a built-in environment-responsive drug release feature: once in lysosomes, the loaded drug molecules are released instantly (<1 min) and completely (∼100 %). Our PNCAS-based drug delivery system is spontaneously formed by simple mixing of hydrophobic nanoparticles, albumin and drugs. Several issues related to industrial production are studied. The ultrahigh drug loading and stability of DOX-loaded PNCAS enabled the delivery of an exceptionally high dose of DOX into a mouse model of breast cancer, yielding high efficacy and no observed toxicity. With further developments, our PNCAS-based delivery systems could serve as a platform technology to meet the multiple requirements of clinical translation of nanomedicines.


Subject(s)
Doxorubicin , Drug Liberation , Lysosomes , Nanoparticles , Doxorubicin/administration & dosage , Doxorubicin/chemistry , Doxorubicin/pharmacokinetics , Animals , Nanoparticles/chemistry , Female , Drug Carriers/chemistry , Mice , Colloids/chemistry , Humans , Drug Delivery Systems , Mice, Inbred BALB C , Drug Stability , Antibiotics, Antineoplastic/administration & dosage , Antibiotics, Antineoplastic/chemistry , Antibiotics, Antineoplastic/pharmacokinetics , Cell Line, Tumor , Breast Neoplasms/drug therapy
15.
Biomacromolecules ; 25(6): 3840-3849, 2024 Jun 10.
Article in English | MEDLINE | ID: mdl-38801711

ABSTRACT

The associative phase separation of charged biomacromolecules plays a key role in many biophysical events that take place in crowded intracellular environments. Such natural polyelectrolyte complexation and phase separation often occur at nonstoichiometric charge ratios with the incorporation of bioactive proteins, which is not studied as extensively as those complexations at stoichiometric ratios. In this work, we investigated how the addition of a crowding agent (polyethylene glycol, PEG) affected the complexation between chitosan (CS) and hyaluronic acid (HA), especially at nonstoichiometric ratios, and the encapsulation of enzyme (catalase, CAT) by the colloidal complexes. The crowded environment promoted colloidal phase separation at low charge ratios, forming complexes with increased colloidal and dissolution stability, which resulted in a smaller size and polydispersity (PDI). The binding isotherms revealed that the addition of PEG greatly enhanced the ion-pairing strength (with increased ion-pairing equilibrium constant Ka from 4.92 × 104 without PEG to 1.08 × 106 with 200 g/L PEG) and switched the coacervation from endothermic to exothermic, which explained the promoted complexation and phase separation. At the stoichiometric charge ratio, the enhanced CS-HA interaction in crowded media generated a more solid-like coacervate phase with a denser network, slower chain relaxation, and higher modulus. Moreover, both crowding and complex encapsulation enhanced the activity and catalytic efficiency of CAT, represented by a 2-fold increase in catalytic efficiency (Kcat/Km) under 100 g/L PEG crowding and CS-HA complex encapsulation. This is likely due to the lower polarity in the microenvironment surrounding the enzyme molecules. By a systematic investigation of both nonstoichiometric and stoichiometric charge ratios under macromolecular crowding, this work provided new insights into the complexation between natural polyelectrolytes in a scenario closer to an intracellular environment.


Subject(s)
Catalase , Chitosan , Hyaluronic Acid , Polyethylene Glycols , Hyaluronic Acid/chemistry , Chitosan/chemistry , Polyethylene Glycols/chemistry , Catalase/chemistry , Colloids/chemistry
16.
Environ Sci Technol ; 58(19): 8531-8541, 2024 May 14.
Article in English | MEDLINE | ID: mdl-38690765

ABSTRACT

Colloidal activated carbon (CAC) is an emerging technology for the in situ remediation of groundwater impacted by per- and polyfluoroalkyl substances (PFAS). In assessing the long-term effectiveness of a CAC barrier, it is crucial to evaluate the potential of emplaced CAC particles to be remobilized and migrate away from the sorptive barrier. We examine the effect of two polymer stabilizers, carboxymethyl cellulose (CMC) and polydiallyldimethylammonium chloride (PolyDM), on CAC deposition and remobilization in saturated sand columns. CMC-modified CAC showed high mobility in a wide ionic strength (IS) range from 0.1 to 100 mM, which is favorable for CAC delivery at a sufficient scale. Interestingly, the mobility of PolyDM-modified CAC was high at low IS (0.1 mM) but greatly reduced at high IS (100 mM). Notably, significant remobilization (release) of deposited CMC-CAC particles occurred upon the introduction of solution with low IS following deposition at high IS. In contrast, PolyDM-CAC did not undergo any remobilization following deposition due to its favorable interactions with the quartz sand. We further elucidated the CAC deposition and remobilization behaviors by analyzing colloid-collector interactions through the application of Derjaguin-Landau-Verwey-Overbeek theory, and the inclusion of a discrete representation of charge heterogeneity on the quartz sand surface. The classical colloid filtration theory was also employed to estimate the travel distance of CAC in saturated columns. Our results underscore the roles of polymer coatings and solution chemistry in CAC transport, providing valuable guidelines for the design of in situ CAC remediation with maximized delivery efficiency and barrier longevity.


Subject(s)
Colloids , Environmental Restoration and Remediation , Groundwater , Groundwater/chemistry , Colloids/chemistry , Environmental Restoration and Remediation/methods , Polymers/chemistry , Charcoal/chemistry , Sand/chemistry , Water Pollutants, Chemical/chemistry , Carbon/chemistry
17.
Environ Pollut ; 353: 124150, 2024 Jul 15.
Article in English | MEDLINE | ID: mdl-38735466

ABSTRACT

In the environment, soil colloids are widespread and possess a significant adsorption capacity. This makes them capable of transporting different pollutants, presenting a potential risk to human and ecological well-being. This study aimed to examine the adsorption and co-migration characteristics of benzo(a)pyrene (BaP) and soil colloids in areas contaminated with organic substances, utilizing both static and dynamic batch experiments. In the static adsorption experiments, it was observed that the adsorption of BaP onto soil colloids followed the pseudo-second-order kinetic model (R2 = 0.966), and the adsorption isotherm conformed to the Langmuir model (R2 = 0.995). The BaP and soil colloids primarily formed bonds through π-π interactions and hydrogen bonds. The dynamic experimental outcomes revealed that elevating colloids concentration contributed to increased BaP mobility. Specifically, when the concentration of soil colloids in influent was 500 mg L-1, the mobility of BaP was 23.2 % compared to that without colloids of 13.4 %. Meanwhile, the lowering influent pH value contributed to increased BaP mobility. Specifically, when the influent pH value was 4.0, the mobility of BaP was 30.1 %. The BaP's mobility gradually declined as the initial concentration of BaP in polluted soil increased. Specifically, when the initial concentration of BaP in polluted soil was 5.27 mg kg-1, the mobility of BaP was 39.1 %. This study provides a support for controlling BaP pollution in soil and groundwater.


Subject(s)
Benzo(a)pyrene , Colloids , Soil Pollutants , Soil , Benzo(a)pyrene/chemistry , Colloids/chemistry , Soil Pollutants/chemistry , Adsorption , Soil/chemistry , Water Pollutants, Chemical/chemistry , Kinetics
18.
Mar Environ Res ; 198: 106553, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38749197

ABSTRACT

The coupling relationship between the <1 kDa, 1-3 kDa, 3-10 kDa, 10-100 kDa, and 100 kDa-0.45 µm Fe fractions and the environmental factors in the Bohai Sea (BS) was investigated. The 1-100 kDa Fe in the surface water exhibited a non-conservative phenomenon during the river-sea mixing process, which was related to the removal of colloidal Fe via flocculation during this process. For the bottom water, the ligands released by the sediments may form additions to the <100 kDa Fe. The COC and DOC were mainly closely related to the behavior of the Fe in the bottom water. The <1 and 3-10 kDa Fe was mainly significantly positively correlated with the DOC, while the <100 kDa-0.45 µm Fe was significantly negatively correlated with the DOC. <100 kDa LMW colloidal Fe exhibited more synergistic behavior with easily absorbed ammonium salts.


Subject(s)
Environmental Monitoring , Iron , Rivers , China , Rivers/chemistry , Iron/chemistry , Iron/analysis , Water Pollutants, Chemical/analysis , Seawater/chemistry , Colloids/chemistry , Geologic Sediments/chemistry , Nutrients/analysis , Oceans and Seas , Water Movements
19.
Adv Colloid Interface Sci ; 329: 103187, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38788307

ABSTRACT

The history of the topic of proteins at soft interfaces dates back to the 19th century, and until the present day, it has continuously attracted great scientific interest. A multitude of experimental methods and theoretical approaches have been developed to serve the research progress in this large domain of colloid and interface science, including the area of soft colloids such as foams and emulsions. From classical methods like surface tension adsorption isotherms, surface pressure-area measurements for spread layers, and surface rheology probing the dynamics of adsorption, nowadays, advanced surface-sensitive techniques based on spectroscopy, microscopy, and the reflection of light, X-rays and neutrons at liquid/fluid interfaces offers important complementary sources of information. Apart from the fundamental characteristics of protein adsorption layers, i.e., surface tension and surface excess, the nanoscale structure of such layers and the interfacial protein conformations and morphologies are of pivotal importance for extending the depth of understanding on the topic. In this review article, we provide an extensive overview of the application of three methods, namely, ellipsometry, X-ray reflectometry and neutron reflectometry, for adsorption and structural studies on proteins at water/air and water/oil interfaces. The main attention is placed on the development of experimental approaches and on a discussion of the relevant achievements in terms of notable experimental results. We have attempted to cover the whole history of protein studies with these techniques, and thus, we believe the review should serve as a valuable reference to fuel ideas for a wide spectrum of researchers in different scientific fields where proteins at soft interface may be of relevance.


Subject(s)
Proteins , Proteins/chemistry , Adsorption , Surface Properties , Water/chemistry , Colloids/chemistry
20.
Food Res Int ; 183: 114223, 2024 May.
Article in English | MEDLINE | ID: mdl-38760142

ABSTRACT

This study investigates the potential of κ-carrageenan hydrogel beads as a delivery system for curcumin, a bioactive compound with various health benefits. Hydrogel beads were prepared using the extrusion technique with a hypodermic needle. The encapsulation efficiency of curcumin in the κ-carrageenan hydrogel beads was found to be 74.61 ± 3.2 %. FTIR spectroscopy analysis revealed shifts in absorption peaks, indicating possible hydrogen bonding and/or ionic interactions between the polymer and salt. An increase in the melting point of curcumin, by 25 °C, in curcumin- κ-carrageenan beads suggests the heat protection offered by the carrageenan chains to curcumin molecules. The in vitro release of curcumin from the beads suggests a sustained and pH-dependent release nature. The release kinetics follow the first order and the Korsmeyer-Peppas model. The outcome offers value-added delivery systems of bioactive compounds toward developing novel food and pharmaceutical applications.


Subject(s)
Carrageenan , Curcumin , Delayed-Action Preparations , Dietary Supplements , Hydrogels , Curcumin/chemistry , Carrageenan/chemistry , Hydrogels/chemistry , Spectroscopy, Fourier Transform Infrared , Hydrogen-Ion Concentration , Drug Liberation , Drug Delivery Systems , Kinetics , Colloids/chemistry , Drug Carriers/chemistry
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