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1.
J Pharm Sci ; 2024 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-39461502

RESUMO

The mechanisms of drug release from amorphous solid dispersions (ASDs) are complex and not fully explored, making it difficult to optimize for in vivo performance. A recurring behavior has been the limit of congruency (LoC), a drug loading above which the ASD surface forms an amorphous drug-rich barrier in the presence of water, which hinders release, especially in non-sink conditions. Drug-polymer interactions and drug glass transition temperature were reported to affect the LoC. However, the effect of polymer molecular weight has not been explored. ASDs of clotrimazole and different molecular weight grades of PVP were studied for their release to obtain their LoC drug loadings. Failure modes underpinning the LoC were investigated using fluorescence confocal microscopy to analyze the ASD/solution interface and phase behavior of ASD films at high relative humidity. ASDs with good release formed stable drug-rich nanodroplets at the ASD/solution interface, while ASDs with poor release were limited by one of two failure modes, depending on PVP molecular weight. In Failure Mode I the nanodroplets quickly agglomerated, while in Failure Mode II the system underwent phase inversion. This work highlights the importance of identifying the mechanisms underlying the LoC to improve the release of higher drug loading ASDs.

2.
Heliyon ; 10(16): e36215, 2024 Aug 30.
Artigo em Inglês | MEDLINE | ID: mdl-39247311

RESUMO

Various industries polluting the water bodies by discharging untreated wastewater directly into the environment and conventional wastewater treatments are often insufficient for effectively treating the pollutants. However, membrane bioreactors (MBRs) offer a promising solution for wastewater treatment where membrane serving as the heart of the system. In this study, polyethersulfone (PES) was used as the membrane material and hydrophilicity of the membranes were tuned up by mixing with hydrophilic additives such as polyethylene glycol (PEG) and polyvinylpyrrolidone (PVP) and the membranes have shown promising results in treating wastewater, particularly in terms of chemical oxygen demand (COD), biochemical oxygen demand (BOD), and color removal. For example, PES-PEG membrane demonstrated COD, BOD, and color removal of 96 %, 94 %, and 92 %, respectively while those were 95 %, 94 %, and 92 %, respectively for PES-based commercial membrane. Although the performances of fabricated membranes were comparable to that of commercial membrane in COD, BOD, and color removal efficiencies, there is room for improvement in permeate yields. Notably, the average permeate efficiency for MBR modules produced with PES-3PEG and PES-5PVP membranes was recorded as 47 % (18 L/m2h) and 13 % (5 L/m2h) respectively of the commercial membrane (38 L/m2h). Despite the variance in permeate yields, the fabricated membranes also showcased significant efficacy in removing microorganisms, a crucial aspect of wastewater treatment. Their performance in this regard proved highly comparable to that of the commercial membrane, emphasizing the potential of these fabricated membranes in enhancing the wastewater treatment.

3.
ACS Nano ; 18(37): 25499-25511, 2024 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-39228057

RESUMO

Pickering emulsions (PEs) are stabilized by particles at the water/oil interface and exhibit superior long-term stability compared to emulsions with molecular surfactants. Among colloidal stabilizers, nano/microgels facilitate emulsification and can introduce stimuli responsiveness. While increasing their hydrophobicity is connected to phase inversion from oil-in-water (O/W) to water-in-oil (W/O) emulsions, a predictive model to relate this phase inversion to the molecular structure of the nano/microgel network remains missing. Addressing this challenge, we developed a library of amphiphilic nanogels (ANGs) that enable adjusting their hydrophobicity while maintaining similar colloidal structures. This enabled us to systematically investigate the influence of network hydrophobicity on emulsion stabilization. We found that W/O emulsions are preferred with increasing ANG hydrophobicity, oil polarity, and oil/water ratio. For nonpolar oils, increasing emulsification temperature enabled the formation of W/O PEs that are metastable at room temperature. We connected this behavior to interfacial ANG adsorption kinetics and quantified ANG deformation and swelling in both phases via atomic force microscopy. Importantly, we developed a quantitative method to predict phase inversion by the difference in Flory-Huggins parameters between ANGs with water and oil (χwater - χoil). Overall, this study provides crucial structure-property relations to assist the design of nano/microgels for advanced PEs.

4.
Environ Sci Pollut Res Int ; 31(40): 53424-53436, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-39190248

RESUMO

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


Assuntos
Hidrogênio , Membranas Artificiais , Polivinil , Zeolitas , Polivinil/química , Zeolitas/química , Hidrogênio/química , Permeabilidade , Polímeros/química , Imidazóis/química , Polímeros de Fluorcarboneto
5.
Chemosphere ; 364: 143170, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39181464

RESUMO

Microplastics (MPs) and other organic matters in textile wastewater have posed a formidable challenge for treatment processes, particularly in the primary stages such as ultrafiltration (UF). UF plays a crucial role in preventing the entry of pollutants into subsequent treatment steps. However, the performance efficiency of UF membranes is compromised by the potential fouling of membrane pores by MPs, dyes and other organic pollutants such as bovine serum albumin (BSA). This study focuses on enhancing UF membrane performance, specifically its antifouling properties, through the development of high-performance membranes using MIL-53(Fe) metal-organic framework (MOF) particles (noted as MIL-53 here). Various concentrations of the MIL-53 (0.05, 0.1, 0.2, and 0.5 wt%) were integrated into the membrane structure through phase inversion process. Streaming zeta potential results confirmed the negatively charged surface of the membranes and their high hydrophilicity was validated through contact angle analysis. FTIR, SEM, EDS, and XRD confirmed the presence of MIL-53 particles on the surface of membranes. The developed membranes were tested for 24 h to assess their antifouling properties, with a subsequent 30-min hydraulic flush to measure their flux recovery ratios. Methylene Blue (MB) dye was used as a cationic dye present in textile wastewater to evaluate the efficiency of the developed membranes in dye removal and the synergistic effects of dye rejection in the presence of organic matters (i.e., MPs and BSA). Since previous studies have not fully addressed the combination of dyes and organic matter, this study thoroughly investigated the effect of particle-type foulants (MPs) and their interactions with dye (MB), as well as water soluble protein-type foulants (BSA) and their interaction with MB. The results indicated that the developed membranes exhibited higher MB rejection when the dye was present with either MP or BSA, along with improved antifouling properties. The optimised UF membrane integrated with 0.1 wt% MIL-53 demonstrated nearly 96% BSA rejection and around 86% MB rejection in the mixed foulant case (BSA-MB). The modified membrane exhibited a substantial increase in water flux from 176 L m-2.h-1 to 327 L m-2.h-1. The findings of this research show the potential of iron-based MOFs in improving the performance of UF membranes and provide a platform for future studies on significant areas such as long-term stability studies and testing with other pollutants found in textile wastewater.


Assuntos
Corantes , Membranas Artificiais , Estruturas Metalorgânicas , Microplásticos , Ultrafiltração , Eliminação de Resíduos Líquidos , Águas Residuárias , Poluentes Químicos da Água , Ultrafiltração/métodos , Águas Residuárias/química , Corantes/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Estruturas Metalorgânicas/química , Eliminação de Resíduos Líquidos/métodos , Microplásticos/química , Têxteis , Purificação da Água/métodos , Indústria Têxtil
6.
ACS Appl Mater Interfaces ; 16(34): 44863-44878, 2024 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-39136722

RESUMO

Separators play a critical role in lithium-ion batteries (LIBs) by facilitating lithium-ion (Li-ion) transport while enabling safe battery operation. However, commercial separators made from polypropylene (PP) or polyethylene (PE) impose a discrete processing step in current LIB manufacturing as they cannot be manufactured with the same slot-die coating process used to fabricate the electrodes. Moreover, commercial separators cannot accommodate newer manufacturing processes used to produce leading-edge microbatteries and flexible batteries with customized form factors. As a path toward rethinking LIB fabrication, we have developed a high-viscosity polymer composite separator slurry that enables the fabrication of both freestanding and direct-on-electrode films. A streamlined phase inversion process is used to impart porosity in cast separator films upon drying. To understand the impacts of material composition and rheology on phase inversion processing and separator performance, we investigated four different separator formulations. We used either diethylene glycol (DEG) or triethyl phosphate (TEP) as a nonsolvent, and either silica (SiO2) or alumina (Al2O3) as an inorganic additive in a polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) matrix. Through a down-selection process, we developed a TEP-SiO2 separator formulation that matched or outperformed a commercial Celgard 2325 (PP/PE/PP) separator and a Beyond Battery ceramic-coated PE (CC/PE/CC) separator under rate and cycle life tests in LiFePO4|Li4Ti5O12 (LFP|LTO) and LiNi0.5Mn0.3Co0.2O2|graphite (NMC-532|graphite) coin cells at C/10-1C rates. Our TEP-SiO2 slurry had a viscosity of 298 Pa s at a 1 s-1 shear rate and shear-thinning behavior. When deposited directly onto an LTO anode and cycled against an LFP cathode, the direct-on-electrode TEP-SiO2 separator increased the specific capacity by 58% and 304% at 2C rates relative to the PP/PE/PP and CC/PE/CC separators, respectively. Additionally, the freestanding TEP-SiO2 separator maintained dimensional stability when heated to 200 °C for 1 h and demonstrated a higher elastic modulus and hardness than the PP/PE/PP and CC/PE/CC separators when measured with nanoindentation.

7.
Int J Biol Macromol ; 277(Pt 4): 134540, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39111465

RESUMO

Algal proteins are an emerging source of functional foods. Herein, Chlorella pyrenoidosa protein (CPP)/xanthan gum-based hydrogels (HG) and beeswax-gelled oleogels (OG) are adopted to fabricate bigels. The phase inversion of bigels can be regulated by the ratio of OG and HG: As the OG increased, bigels turn from OG-in-HG (OG/HG) to a semicontinuous state and then HG-in-OG (HG/OG). In OG/HG bigels (OG ≤ 50 %), hydrophilic CPP acts as the emulsifier at the interface of OG and HG, while beeswax emulsifies the system in HG/OG bigels (OG = 80 %). A semicontinuous bigel appears during the transition between HG/OG and OG/HG. The increase of OG can enhance the viscoelasticity, hardness, adhesiveness, chewiness, and thermal stability. OG/HG bigels exhibit stronger thixotropic recovery and oil-holding capacity than HG/OG bigels. In the in-vitro digestion and food 3D printing, the high specific surface area and the highest thixotropic recovery caused by the emulsion structure of the OG/HG bigel (OG = 50 %) are conducive to the release of free fatty acids and molding of 3D-printed objects, respectively. This study provides a new approach to structure the gelled water-oil system with CPP and helps to develop edible algal proteins-based multiphase systems in food engineering or pharmacy.


Assuntos
Chlorella , Impressão Tridimensional , Ceras , Ceras/química , Chlorella/química , Hidrogéis/química , Digestão , Compostos Orgânicos/química , Emulsões/química , Proteínas de Algas/química , Proteínas de Algas/metabolismo
8.
Materials (Basel) ; 17(13)2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38998448

RESUMO

Waterborne polyurethane asphalt emulsion (WPUA) is an environmentally friendly bituminous material, whose performance is highly dependent on the phase structure of the continuous phase. In this paper, WPUAs in the vicinity of phase inversion were prepared using waterborne polyurethane (WPU) and asphalt emulsion. The chemical structures, thermal stability, dynamic mechanical properties, phase-separated morphology and mechanical performance of WPUAs were studied. Fourier-transform infrared (FTIR) spectra revealed that there are no -NCO bonds in either the pure WPU or WPUAs. Moreover, the preparation of WPUA is a physical process. The addition of WPU weakens the thermal stability of asphalt emulsion. WPU improves the storage modulus of asphalt emulsion at lower and higher temperatures. The glass transition temperatures of the WPUA films are higher than that of the pure WPU film. When the WPU concentration increases from 30 wt% to 40 wt%, phase inversion occurs; that is, the continuous phase shifts from asphalt to WPU. The WPUA films have lower tensile strength and toughness than the pure WPU film. However, the elongations at break of the WPUA films are higher than that of the pure WPU film. Both the tensile strength and toughness of the WPUA films increase with the WPU concentration. Due to the occurrence of phase inversion, the elongation at break, tensile strength and toughness of the WPUA film containing 30 wt% WPU are increased by 29%, 250% and 369%, respectively, compared to the film with 40 wt% WPU.

9.
Int J Biol Macromol ; 277(Pt 2): 134170, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39067731

RESUMO

Agricultural waste presents a significant environmental challenge due to improper disposal and management practices, contributing to soil degradation, biodiversity loss, and pollution of water and air resources. To address these issues, there is a growing emphasis on the valorization of agricultural waste. Cellulose, a major component of agricultural waste, offers promising opportunities for resource utilization due to its unique properties, including biodegradability, biocompatibility, and renewability. Thus, this review explored various types of agricultural waste, their chemical composition, and pretreatment methods for cellulose extraction. It also highlights the significance of rice straw, sugarcane bagasse, and other agricultural residues as cellulose-rich resources. Among the various membrane fabrication techniques, phase inversion is highly effective for creating porous membranes with controlled thickness and uniformity, while electrospinning produces nanofibrous membranes with high surface area and exceptional mechanical properties. The review further explores the separation of pollutants including using cellulose membranes, demonstrating their potential in environmental remediation. Hence, by valorizing agricultural residues into functional materials, this approach addresses the challenge of agricultural waste management and contributes to the development of innovative solutions for pollution control and water treatment.


Assuntos
Agricultura , Celulose , Membranas Artificiais , Celulose/química , Agricultura/métodos , Biodegradação Ambiental , Poluentes Ambientais/química , Poluentes Ambientais/isolamento & purificação
10.
ACS Nano ; 18(26): 16895-16904, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38906832

RESUMO

Particulate matter (PM) pollution has posed a serious threat to public health, especially the global spread of infectious diseases. Most existing air filtration materials are still subjected to a compromise between removal efficiency and air permeability on account of their stacking bulk structures. Here, we proposed a self-polarized assembly technique to create two-dimensional piezoelectric nanofibrous webs (PNWs) directly from polymer solutions. The strategy involves droplets deforming into ultrathin liquid films by inertial flow, liquid films evolving into web-like architectures by instantaneous phase inversion, and enhanced dipole alignment by cluster electrostatics. The assembled continuous webs exhibit integrated structural superiorities of nanoscale diameters (∼20 nm) of the internal fibers and through pores (∼100 nm). Combined with the wind-driven electrostatic property derived from the enhanced piezoelectricity, the PNW filter shows high efficiency (99.48%) and low air resistance (34 Pa) against PM0.3 as well as high transparency (84%), superlight weight (0.7 g m-2), and long-term stable service life. This creation of such versatile nanomaterials may offer insight into the design and upgrading of high-performance filters.

11.
Drug Deliv Transl Res ; 14(12): 3494-3511, 2024 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38739319

RESUMO

Brain drug delivery is severely hindered by the presence of the blood-brain barrier (BBB). Its functionality relies on the interactions of the brain endothelial cells with additional cellular constituents, including pericytes, astrocytes, neurons, or microglia. To boost brain drug delivery, nanomedicines have been designed to exploit distinct delivery strategies, including magnetically driven nanocarriers as a form of external physical targeting to the BBB. Herein, a lipid-based magnetic nanocarrier prepared by a low-energy method is first described. Magnetic nanocapsules with a hydrodynamic diameter of 256.7 ± 8.5 nm (polydispersity index: 0.089 ± 0.034) and a ξ-potential of -30.4 ± 0.3 mV were obtained. Transmission electron microscopy-energy dispersive X-ray spectroscopy analysis revealed efficient encapsulation of iron oxide nanoparticles within the oily core of the nanocapsules. Both thermogravimetric analysis and phenanthroline-based colorimetric assay showed that the iron oxide percentage in the final formulation was 12 wt.%, in agreement with vibrating sample magnetometry analysis, as the specific saturation magnetization of the magnetic nanocapsules was 12% that of the bare iron oxide nanoparticles. Magnetic nanocapsules were non-toxic in the range of 50-300 µg/mL over 72 h against both the human cerebral endothelial hCMEC/D3 and Human Brain Vascular Pericytes cell lines. Interestingly, higher uptake of magnetic nanocapsules in both cell types was evidenced in the presence of an external magnetic field than in the absence of it after 24 h. This increase in nanocapsules uptake was also evidenced in pericytes after only 3 h. Altogether, these results highlight the potential for magnetic targeting to the BBB of our formulation.


Assuntos
Barreira Hematoencefálica , Lipídeos , Nanopartículas Magnéticas de Óxido de Ferro , Nanocápsulas , Barreira Hematoencefálica/metabolismo , Nanopartículas Magnéticas de Óxido de Ferro/química , Nanopartículas Magnéticas de Óxido de Ferro/administração & dosagem , Nanocápsulas/química , Lipídeos/química , Lipídeos/administração & dosagem , Humanos , Sistemas de Liberação de Medicamentos , Portadores de Fármacos/química , Portadores de Fármacos/farmacocinética , Portadores de Fármacos/administração & dosagem , Células Endoteliais/metabolismo , Tamanho da Partícula
12.
Chemosphere ; 357: 141982, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38608778

RESUMO

Powdered activated carbon (PAC) has been extensively used as an effective adsorbent. Despite its excellent adsorption ability, PAC has drawbacks, including difficulty in filtration and reactivation after use, limitations of mass transfer in deeper areas because of its aggregated powder form, and limited applicability in high-flow systems. To overcome these limitations, we used a three-dimensional (3D) printing system to fabricate PAC into a 3D structure. Spectral and microscopic analyses indicated that PAC was embedded into 3D monolith and exhibited high porosity suitable for facile mass transfer. The designed 3D PAC filter effectively removed 200 ppm-methylene blue (MB) within 8 h and showed an adsorption efficiency of 93.4 ± 0.9%. The adsorption of MB onto the 3D PAC filter was described by the pseudo-first-order kinetic and Freundlich isotherm models. The negatively charged 3D PAC filter might attract the positively charged MB, thus favoring the physical adsorption of MB onto the 3D PAC filter. The adsorption performance of the 3D PAC filter was tested at various pH levels of 4-10 and against MB spiked in seawaters and freshwaters to evaluate its feasibility for use in real environments. Finally, the reproducibility and reusability of the 3D PAC filter were demonstrated through repeated adsorption and desorption processes against MB.


Assuntos
Carvão Vegetal , Corantes , Azul de Metileno , Impressão Tridimensional , Poluentes Químicos da Água , Purificação da Água , Carvão Vegetal/química , Adsorção , Corantes/química , Poluentes Químicos da Água/química , Azul de Metileno/química , Purificação da Água/métodos , Pós , Cinética , Cátions/química , Filtração/métodos , Porosidade , Carbono/química , Concentração de Íons de Hidrogênio
13.
Int J Biol Macromol ; 266(Pt 2): 131102, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38580021

RESUMO

Sericin protein possesses excellent biocompatibility, antioxidation, and processability. Nevertheless, manufacturing large quantities of strong and tough pure regenerated sericin materials remains a significant challenge. Herein, we design a lightweight structural sericin film with high ductility by combining radical chain polymerization reaction and liquid-solid phase inversion method. The resulting polyacrylonitrile grafted sericin films exhibit the ability to switch between high strength and high toughness effortlessly, the maximum tensile strength and Young's modulus values are 21.92 ± 1.51 MPa and 8.14 ± 0.09 MPa, respectively, while the elongation at break and toughness reaches up to 344.10 ± 35.40 % and 10.84 ± 1.02 MJ·m-3, respectively. Our findings suggest that incorporating sericin into regenerated films contributes to the transformation of their mechanical properties through influencing the entanglement of molecular chains within polymerized solutions. Structural analyses conducted using infrared spectroscopy and X-ray diffraction confirm that sericin modulates the mechanical properties by affecting the transition of condensed matter conformation. This work presents a convenient yet effective strategy for simultaneously addressing the recycling of sericin as well as producing regenerated protein-based films that hold potential applications in biomedical, wearable, or food packaging.


Assuntos
Resinas Acrílicas , Reologia , Sericinas , Sericinas/química , Resinas Acrílicas/química , Resistência à Tração , Fenômenos Mecânicos , Polimerização , Soluções , Módulo de Elasticidade , Difração de Raios X
14.
Membranes (Basel) ; 14(4)2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38668119

RESUMO

Zeolite serves as a promising additive for enhancing the hydrophilicity of polymeric membranes, yet its utilization for bolstering the mechanical strength of the membrane remains limited. In this study, poly(vinylidene fluoride) (PVDF) membranes were modified by incorporating various concentrations of zeolite (0.5-2 wt%) to improve not only their mechanical properties, but also other features for water filtration. Membranes with and without zeolite incorporation were fabricated via a dry-wet phase inversion technique, followed by the application of a series of characterization techniques in order to study their morphological structure, mechanical strength, and hydrophilicity. The membrane filtration performance for each membrane was evaluated based on pure water flux and Bovine Serum Albumin (BSA) rejection. Field-Emission Scanning Electron Microscopy (FESEM) images revealed a dense, microvoid-free structure across all of the PVDF membranes, contributing to a high pristine PVDF membrane tensile strength of 14 MPa. The addition of 0.5 wt% zeolite significantly improved the tensile strength up to 19.4 MPa. Additionally, the incorporation of 1 wt% zeolite into PVDF membrane yielded improvements in membrane hydrophilicity (contact angle of 67.84°), pure water flux (63.49% increase), and high BSA rejection (95.76%) compared to pristine PVDF membranes. To further improve the characterization of the zeolite-modified PVDF membranes, the Support Vector Regression (SVR) model was adopted to estimate the molecular weight cut off (MWCO) of the membranes. A coefficient of determination (R2) value of 0.855 was obtained, suggesting that the SVR model predicted the MWCO accurately. The findings of this study showed that the utilization of zeolite is promising in enhancing both the mechanical properties and separation performance of PVDF membranes for application in ultrafiltration processes.

15.
ACS Appl Mater Interfaces ; 16(14): 17411-17421, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38557056

RESUMO

Over the past decade, direct air capture (DAC) of carbon dioxide (CO2) using solid nanoadsorbents has garnered attention as a negative emission technology with high energy efficiency. Although operational, the large-scale deployment of DAC technologies has been significantly delayed due to the low performance and high cost of solid DAC nanoadsorbents. Herein, we present a novel family of meso-macroporous melamine formaldehyde (MF) materials with a facile preparation methodology, low capital cost, and unique physicochemical characteristics for DAC. The fabricated MF materials exhibit an extra-large pore volume of 5.19 cm3/g with a 24.6 nm average pore diameter. We show that the synthesized MF materials can be used as substrates and impregnated with different amounts of tetraethylenepentamine (TEPA) to act as chemical nanoadsorbents for DAC. Owing to the ultrahigh pore volume of MF, a substantial amount of 71 wt % TEPA (i.e., MF-TEPA71%) can be loaded, resulting in 2.65 mmol/g of CO2 uptake under DAC conditions. In addition, the superior physicochemical properties of MF lead to a high CO2 loading of 2.07 mmol/g with low TEPA loading in MF-TEPA33%. The prepared MF-TEPA nanoadsorbents can be successfully employed in different shapes (i.e., droplets, pellets, and coatings) and maintain their superiority across different temperatures and CO2 concentrations. This study provides a promising approach for developing meso-macroporous substrates through a straightforward and scalable synthesis method, representing a new avenue for the next generation of DAC nanoadsorbents with superior performance for practical applications.

16.
Mol Pharm ; 21(4): 1900-1918, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38469754

RESUMO

The use of amorphous solid dispersions (ASDs) in commercial drug products has increased in recent years due to the large number of poorly soluble drugs in the pharmaceutical pipeline. However, the release behavior of ASDs is complex and remains not well understood. Often, the drug release from ASDs is rapid and complete at lower drug loadings (DLs) but becomes slow and incomplete at higher DLs. The DL where release becomes hindered is termed the limit of congruency (LoC). Currently, there are no approaches to predict the LoC. However, recent findings show that one potential cause leading to the LoC is a change in phase morphology after water-induced phase separation at the ASD/solution interface. In this study, the phase behavior of ASDs in contact with aqueous solutions was described thermodynamically by constructing experimental and computational ternary phase diagrams, and these were used to predict morphology changes and ultimately the LoC. Experimental ternary phase diagrams were obtained by equilibrating ASD/water mixtures over time. Computational ternary phase diagrams were obtained by Perturbed Chain Statistical Associating Fluid Theory (PC-SAFT). The morphology of the hydrophobic phase was studied with fluorescence confocal microscopy. It was demonstrated that critical point (plait point) composition approximately corresponded to the ASD DL, where the hydrophobic phase, formed during phase separation, became interconnected and hindered ASD release. This work provides mechanistic insights into the ASD release behavior and highlights the potential of in silico ASD design using phase diagrams.


Assuntos
Água , Solubilidade , Liberação Controlada de Fármacos , Água/química , Interações Hidrofóbicas e Hidrofílicas , Composição de Medicamentos
17.
Molecules ; 29(5)2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38474660

RESUMO

In this study, novel amphiphilic polymer emulsifiers for avermectin (Avm) were synthesized facilely via the hydrolysis of ethylene-maleic anhydride copolymer (EMA) with different agents, and their structures were confirmed by various techniques. Then, water-based Avm-nanoemulsions were fabricated with the emulsifiers via phase inversion emulsification process, and superior emulsifier was selected via the emulsification effects. Using the superior emulsifier, an optimal Avm-nanoemulsion (defined as Avm@HEMA) with satisfying particle size of 156.8 ± 4.9 nm, encapsulation efficiency (EE) of 69.72 ± 4.01% and drug loading capacity (DLC) of 54.93 ± 1.12% was constructed based on response surface methodology (RSM). Owing to the emulsifier, the Avm@HEMA showed a series of advantages, including high stability, ultraviolet resistance, low surface tension, good spreading and high affinity to different leaves. Additionally, compared to pure Avm and Avm-emulsifiable concentrate (Avm-EC), Avm@HEMA displayed a controlled releasing feature. The encapsulated Avm was released quite slowly at normal conditions (pH 7.0, 25 °C or 15 °C) but could be released at an accelerated rate in weak acid (pH 5.5) or weak alkali (pH 8.5) media or at high temperature (40 °C). The drug releasing profiles of Avm@HEMA fit the Korsmeyer-Peppas model quite well at pH 7.0 and 25 °C (controlled by Fickian diffusion) and at pH 7.0 and 10 °C (controlled by non-Fickian diffusion), while it fits the logistic model under other conditions (pH 5.5 and 25 °C, pH 8.5 and 25 °C, pH 7.0 and 40 °C).

18.
J Magn Reson ; 361: 107653, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38471414

RESUMO

Nuclear magnetic resonance (NMR) based 13C tracing has broad applications across medical and environmental research. As many biological and environmental samples are heterogeneous, they experience considerable spectral overlap and relatively low signal. Here a 1D 1H-12C/13C is introduced that uses "in-phase/opposite-phase" encoding to simultaneously detect and discriminate both protons attached to 12C and 13C at full 1H sensitivity in every scan. Unlike traditional approaches that focus on the 12C/13C satellite ratios in a 1H spectrum, this approach creates separate sub-spectra for the 12C and 13C bound protons. These spectra can be used for both quantitative and qualitative analysis of complex samples with significant spectral overlap. Due to the presence of the 13C dipole, faster relaxation of the 1H-13C pairs results in slight underestimation compared to the 1H-12C pairs. However, this is easily compensated for, by collecting an additional reference spectrum, from which the absolute percentage of 13C can be calculated by difference. When combined with the result, 12C and 13C percent enrichment in both 1H-12C and 1H-13C fractions are obtained. As the approach uses isotope filtered 1H NMR for detection, it retains nearly the same sensitivity as a standard 1H spectrum. Here, a proof-of-concept is performed using simple mixtures of 12C and 13C glucose, followed by suspended algal cells with varying 12C /13C ratios representing a complex mixture. The results consistently return 12C/13C ratios that deviate less than 1 % on average from the expected. Finally, the sequence was used to monitor and quantify 13C% enrichment in Daphnia magna neonates which were fed a 13C diet over 1 week. The approach helped reveal how the organisms utilized the 12C lipids they are born with vs. the 13C lipids they assimilate from their diet during growth. Given the experiments simplicity, versatility, and sensitivity, we anticipate it should find broad application in a wide range of tracer studies, such as fluxomics, with applications spanning various disciplines.


Assuntos
Isótopos , Prótons , Espectroscopia de Ressonância Magnética/métodos , Misturas Complexas , Lipídeos
19.
AAPS PharmSciTech ; 25(2): 32, 2024 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-38332361

RESUMO

Bacterial cellulose (BC) is an interesting material for drug delivery applications due to its high purity. This study aimed to compare the properties of tablets prepared by the wet granulation method using bacterial cellulose prepared by different methods as a diluent, using acetaminophen as a model drug. BC used as diluents were prepared using two different methods: freeze-drying (BC-FD) and phase-inversion (BC-PI), and their characteristics were analyzed and compared with that of commercial microcrystalline cellulose PH 101 (Comprecel® M101). Acetaminophen tablets were prepared by wet granulation using BC-FD, BC-PI, or Comprecel® M101 as diluents, and their tablet properties were examined. The result showed that the morphology, polymorph, and crystallinity of BC-PI and Comprecel® M101 were similar but they were different compared with that of BC-FD. Tablets could be successfully formed using BC-PI and Comprecel® M101 as diluents without any physical defects but the tablet prepared using BC-FD as diluent appeared chipped edge. The characteristics (thickness, weight variation, hardness, friability, disintegration, drug content, and dissolution) of the tablets prepared using BC-PI diluent were also similar to those prepared using Comprecel® M101 diluent, but those of BC-FD diluent were inferior. This indicates that BC prepared in BC-PI can potentially be used as a diluent for tablets prepared by wet granulation.


Assuntos
Acetaminofen , Celulose , Acetaminofen/química , Celulose/química , Solubilidade , Excipientes/química , Comprimidos/química
20.
Polymers (Basel) ; 16(3)2024 Feb 04.
Artigo em Inglês | MEDLINE | ID: mdl-38337323

RESUMO

Poly(D,L-lactide-co-glycolide is a biodegradable copolymer that can release pharmaceuticals. These pharmaceuticals can provide local therapy and also avert the clinical issues that occur when a drug must be given continuously and/or automatically. However, the drawbacks of using poly(D,L-lactide-co-glycolide include the kinetics and duration of time of poly(D,L-lactide-co-glycolide drug release, the denaturing of the drug loaded drug, and the potential clinical side effects. These drawbacks are mainly caused by the volatile organic solvents needed to prepare poly(D,L-lactide-co-glycolide spheres. Using the non-toxic solvent glycofurol solvent instead of volatile organic solvents to construct poly(D,L-lactide-co-glycolide microspheres may deter the issues of using volatile organic solvents. Up to now, preparation of such glycofurol spheres has previously met with limited success. We constructed dexamethasone laden poly(D,L-lactide-co-glycolide microspheres utilizing glycofurol as the solvent within a modified phase inversion methodology. These prepared microspheres have a higher drug load and a lower rate of water diffusion. This prolongs drug release compared to dichloromethane constructed spheres. The glycofurol-generated spheres are also not toxic to target cells as is the case for dichloromethane-constructed spheres. Further, glycofurol-constructed spheres do not denature the dexamethasone molecule and have kinetics of drug release that are more clinically advantageous, including a lower drug burst and a prolonged drug release.

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