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1.
Biomater Adv ; 164: 213981, 2024 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-39096587

RESUMEN

Generally, oligolysine has poor antibacterial effect and almost no antibacterial activity. Herein, low cost and easily available oligolysines were chosen to prepare injectable antibacterial hydrogel (PVAL-gel) for wound healing. The hydrogel network was formed by cross-linking vanillin acrylate-N, N-dimethylacrylamide copolymer P(VA-co-DMA), oligolysine and adipate dihydrazide through Schiff base bond. The obtained hydrogel PVAL-gel exhibited not only excellent self-healing capability and injectability, but also the efficient contact antibacterial ability and good inhibitory effects on E.coli and S.aureus. In vitro, 99.9 % of pathogenic bacteria was killed within 160 min. Furthermore, the injectable PVAL-gel could rapidly eradicate bacteria in infected wounds and notably enhance the healing of full-thickness skin wounds. Therefore, PVAL-gel is expected to be used as a high-end dressing for the treatment of infected skin wounds, which can promote wound healing.


Asunto(s)
Antibacterianos , Escherichia coli , Hidrogeles , Staphylococcus aureus , Cicatrización de Heridas , Cicatrización de Heridas/efectos de los fármacos , Hidrogeles/química , Hidrogeles/farmacología , Hidrogeles/administración & dosificación , Antibacterianos/farmacología , Antibacterianos/química , Antibacterianos/administración & dosificación , Escherichia coli/efectos de los fármacos , Animales , Staphylococcus aureus/efectos de los fármacos , Benzaldehídos/química , Benzaldehídos/farmacología , Benzaldehídos/administración & dosificación , Pruebas de Sensibilidad Microbiana , Inyecciones , Adipatos/química , Adipatos/farmacología , Ratones , Acrilamidas/química , Acrilamidas/farmacología , Polilisina/química , Polilisina/farmacología
2.
Int J Biol Macromol ; 276(Pt 1): 133786, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38992551

RESUMEN

The poor interfacial compatibility of natural fiber-reinforced polymer composites has become a major challenge in the development of industry-standard high-performance composites. To solve this problem, this study constructs a novel rigid-flexible balanced molecular crosslinked network transition interface in composites. The interface improves the interfacial compatibility of the composites by balancing the stiffness and strength of the fibers and the matrix, effectively improving the properties of the composites. The flexural strength and flexural modulus of the composites were enhanced by 38 % and 44 %, respectively. Water absorption decreased by 30 %. The initial and maximum thermal degradation temperatures increased by 20 °C and 16 °C, respectively. The maximum storage modulus increased by 316 %. Furthermore, the impact toughness was elevated by 41 %, attributed to the crosslinked network's efficacy in absorbing and dissipating externally applied energy. This innovative approach introduces a new theory of interfacial reinforcement compatibility, advancing the development of high-performance and sustainable biocomposites.


Asunto(s)
Materiales Biocompatibles , Materiales Biocompatibles/química , Butadienos/química , Ensayo de Materiales , Reactivos de Enlaces Cruzados/química , Sasa/química , Polímeros/química , Temperatura , Agua/química , Adipatos/química , Resistencia a la Tracción
3.
Biomacromolecules ; 25(8): 4762-4779, 2024 Aug 12.
Artículo en Inglés | MEDLINE | ID: mdl-38989826

RESUMEN

Injectable hydrogels with good antimicrobial and antioxidant properties, self-healing characteristics, suitable mechanical properties, and therapeutic effects have great practical significance for developing treatments for pressing healthcare challenges. Herein, we have designed a novel, self-healing injectable hydrogel composite incorporating cross-linked biofunctional nanomaterials by mixing alginate aldehyde (Ox-Alg), quaternized chitosan (QCS), adipic acid dihydrazide (ADH), and copper oxide nanosheets surface functionalized with folic acid as the bioligand (F-CuO). Gelation was achieved under physiological conditions via the dynamic Schiff base cross-linking mechanism. The developed nanocomposite injectable hydrogel demonstrated the fast self-healing ability essential to bear deformation and outstanding antibacterial properties along with ROS scavenging ability. Furthermore, the optimized formulation of our F-CuO-embedded injectable hydrogel exhibited excellent cytocompatibility, blood compatibility, and in vitro wound healing performance. Taken together, the F-CuO nanosheet cross-linked injectable hydrogel composite presented herein offers a promising candidate biomaterial with multifunctional properties to develop solutions for addressing clinical challenges.


Asunto(s)
Quitosano , Cobre , Hidrogeles , Nanocompuestos , Quitosano/química , Nanocompuestos/química , Hidrogeles/química , Hidrogeles/farmacología , Cobre/química , Cobre/farmacología , Alginatos/química , Cicatrización de Heridas/efectos de los fármacos , Animales , Antibacterianos/farmacología , Antibacterianos/química , Antibacterianos/administración & dosificación , Humanos , Materiales Biocompatibles/química , Materiales Biocompatibles/farmacología , Ácido Fólico/química , Ácido Fólico/farmacología , Adipatos/química , Ratones , Adhesivos/química , Adhesivos/farmacología
4.
Acta Biomater ; 184: 98-113, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38914412

RESUMEN

Postoperative abdominal adhesion (PAA) widely occurs after abdominal surgery, which often produces severe complications. However, there were still no satisfactory anti-adhesive products including barriers and anti-adhesive agents. Herein, we developed a ROS-responsive and scavenging hydrogel barrier, termed AHBC/PSC, wherein the monomer AHBC was synthesized by phenylboronic acid (PBA)-modified hyaluronic acid (HA-PBA) further grafted with adipic dihydrazide (ADH) and PBA-based chlorogenic acid (CGA) via ROS-sensitive borate ester bond, and the other monomer PSC was constructed by polyvinyl alcohol (PVA) grafted with sulfated betaine (SB) and p-hydroxybenzaldehyde (CHO). Further, the double crosslinked AHBC/PSC hydrogel was successfully fabricated between AHBC and PSC via forming dynamic covalent acylhydrazone bonds and borate ester bonds. Results showed that AHBC/PSC hydrogel had in situ gelation behavior, satisfactory mechanical properties (storage modulus of about 1 kPa and loss factor Tan δ of about 0.5), suitable wet tissue adhesion strength of about 2.3 kPa on rat abdominal wall, and good biocompatibility, achieving an ideal physical barrier. Particularly, CGA could be responsively released from the hydrogel by breakage of borate ester bonds between CGA and PBA based on high reactive oxygen species (ROS) levels of damaged tissue and exhibited great ROS scavenging capability to regulate inflammation and promote the polarization of macrophages from pro-inflammatory M1 phenotype to anti-inflammatory M2 phenotype. Moreover, the grafted SB as a zwitterionic group could reduce protein adsorption and fibroblast adhesion. Finally, the in vivo experiments revealed that AHBC/PSC hydrogel with good safety and in vivo retention behavior of about 2 weeks, effectively prevented PAA by regulating the inflammatory microenvironment and alleviating the fibrosis process. In brief, the versatile AHBC/PSC hydrogel would provide a more convenient and efficient approach for PAA prevention. STATEMENT OF SIGNIFICANCE: Postoperative abdominal adhesion (PAA) widely occurs after surgery and is often accompanied by severe complications. Excessive inflammation and oxidative stress are very crucial for PAA formation. This study provides a ROS-responsive and scavenging hydrogel with suitable mechanical properties, good biocompatibility and biodegradability, and resistance to protein and fibroblast. The antioxidant and anti-inflammatory active ingredient could be responsively released from the hydrogel via triggering by the high ROS levels in the postoperative microenvironment thereby regulating the inflammatory balance. Finally, the hydrogel would effectively regulate the development process of PAA thereby achieving non-adhesion wound healing.


Asunto(s)
Hidrogeles , Ratas Sprague-Dawley , Especies Reactivas de Oxígeno , Animales , Adherencias Tisulares/prevención & control , Adherencias Tisulares/patología , Hidrogeles/química , Hidrogeles/farmacología , Especies Reactivas de Oxígeno/metabolismo , Ratas , Ácidos Borónicos/química , Ácido Hialurónico/química , Ácido Hialurónico/farmacología , Complicaciones Posoperatorias/prevención & control , Ratones , Masculino , Depuradores de Radicales Libres/farmacología , Depuradores de Radicales Libres/química , Células RAW 264.7 , Adipatos/química
5.
Pharm Dev Technol ; 29(7): 649-662, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38864367

RESUMEN

The study aimed to fingerprint the physical manufacturing properties of five commonly used acid sources in effervescent systems for designing the formulation and process of such systems. The hygroscopicity, texture properties, rheological torque, compressibility, tabletability, etc., were investigated to inspect 'powder direct compression (DC)' and 'wet granulation and compression' properties of citric (CA), tartaric (TA), malic (MA), fumaric (FA), and adipic acid (AA). The DC ability was evaluated by the SeDeM expert system. The results indicated that all acid powders failed to meet flowability requirements for DC, and plastic deformation dominated during compression. Furthermore, CA exhibited strong hygroscopicity and punch sticking, while MA demonstrated the best tabletability. TA had a large wet granulation space and was relatively the most suitable for DC. AA was extremely hygroscopic, and its flowability improved significantly as particle size increased. Finally, FA displayed the lowest hygroscopicity and ejection force as well as great compressibility and wet granulation space, and did not exhibit punch sticking, while the granule fragments dissolved slowly during disintegration. Generally speaking, the formulation or granulation affected the tabletability, indicating that pairing with other acids or suitable fillers could potentially improve its disadvantages. These multidimensional assessments effectively reduce the pre-exploration and enhance the efficiency of the development of effervescent systems.


Asunto(s)
Composición de Medicamentos , Tamaño de la Partícula , Polvos , Comprimidos , Polvos/química , Composición de Medicamentos/métodos , Excipientes/química , Reología , Humectabilidad , Tartratos/química , Química Farmacéutica/métodos , Malatos/química , Ácidos/química , Fumaratos/química , Adipatos/química , Ácido Cítrico/química
6.
Int J Biol Macromol ; 270(Pt 1): 132076, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38705324

RESUMEN

The cross-linked enzyme (CLEs) of Thermomyces lanuginosa lipase (TLL) was prepared in an isocyanide-based multi-component reactions (ICMRs) platform by applying three di-acidic cross-linkers to unveil more factors contributing to the functional properties of CLEs. The linkers were 1,11-undecanedicarboxylic acid, azelaic acid, and adipic acid with 11, 7, and 4 carbon lengths, respectively, providing a proper tool to investigate the effect of linker length on the activity, stability, and selectivity of the resulting CLEs. The immobilization yields of 60-90 % and the specific activities of 168, 88.4 and 49 U/mg were obtained for the CLEs of 1,11-undecanedicarboxylic acid, azelaic acid, adipic acid, respectively. The lower activity of azelaic and adipic acid-mediated CLEs compared to the soluble TLL (110 U/mg) was explained by in silico calculations. The results revealed that as opposed to 1,11-undecanedicarboxylic acid, both linkers tended to penetrate the enzyme active site, thus resulting in a major inhibitory effect on the enzyme functionality. The thermal and co-solvent stability of the immobilized derivatives improved compared to those of free TLL. The selectivity of CLEs was also examined by catalytic release of main omega-3 fatty acids from fish oil, presenting the highest selectivity of 22 for the CLEs of azelaic acid.


Asunto(s)
Reactivos de Enlaces Cruzados , Enzimas Inmovilizadas , Lipasa , Enzimas Inmovilizadas/química , Enzimas Inmovilizadas/metabolismo , Lipasa/química , Lipasa/metabolismo , Reactivos de Enlaces Cruzados/química , Estabilidad de Enzimas , Eurotiales/enzimología , Adipatos/química , Carbono/química , Ácidos Dicarboxílicos/química
7.
J Hazard Mater ; 472: 134603, 2024 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-38749243

RESUMEN

Polybutylene adipate terephthalic acid (PBAT) is an emerging biodegradable material in food packaging. However, concerns have been raised regarding the potential hazards it could pose to food safety. In this study, the changes of PBAT films during food contact and the release of small molecules were inestigated by a multiscale approach. On a macro-scale, the surface roughness of the films increased with the reduction in the concentration of food simulants and the increase in contact temperatures, especially after immersion in acidic food environments. On a micro-scale, the crystallinity (Xc) and degradation indexes (DI) of the films increased by 5.7-61.2% and 7.8-48.6%, respectively, which led to a decrease in thermal stability. On a scale approaching the molecular level, 2,4-di-tert-butylphenol (2,4-DTBP) was detected by gas chromatography-mass spectrometry (GC-MS/MS) with the highest migration content, and the release behavior of 2,4-DTBP was further investigated by migration kinetics. In addition, terephthalic acid (TPA), a hydrolysis product of PBAT, was detected in acidic food environments by liquid chromatography-mass spectrometry (LC-MS/MS). The results of this study could provide practical guidance and assistance to promote sustainable development in the field of food packaging.


Asunto(s)
Embalaje de Alimentos , Ácidos Ftálicos , Ácidos Ftálicos/química , Poliésteres/química , Adipatos/química , Contaminación de Alimentos/análisis , Cromatografía de Gases y Espectrometría de Masas
8.
Eur J Pharm Biopharm ; 200: 114335, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38768765

RESUMEN

The study endeavors the fabrication of extended-release adipic acid (APA) buccal films employing a quality by design (QbD) approach. The films intended for the treatment of xerostomia were developed utilizing hot-melt extrusion technology. The patient-centered quality target product profile was created, and the critical quality attributes were identified accordingly. Three early-stage formulation development trials, complemented by risk assessment aligned the formulation and process parameters with the product quality standards. Employing a D-optimal mixture design, the formulations were systematically optimized by evaluating three formulation variables: amount of the release-controlling polymer Eudragit® (E RSPO), bioadhesive agent Carbopol® (CBP 971P), and pore forming agent polyethylene glycol (PEG 1500) as independent variables, and % APA release in 1, 4 and 8 h as responses. Using design of experiment software (Design-Expert®), a total of 16 experimental runs were computed and extruded using a Thermofisher ScientificTM twin screw extruder. All films exhibited acceptable content uniformity and extended-release profiles with the potential for releasing APA for at least 8 h. Films containing 30% E RSPO, 10% CBP 971P, and 20% PEG 1500 released 88.6% APA in 8 h. Increasing the CBP concentration enhanced adhesiveness and swelling capacities while decreasing E RSPO concentration yielded films with higher mechanical strength. The release kinetics fitted well into Higuchi and Krosmeyer-Peppas models indicating a Fickian diffusion release mechanism.


Asunto(s)
Preparaciones de Acción Retardada , Liberación de Fármacos , Xerostomía , Xerostomía/tratamiento farmacológico , Tecnología de Extrusión de Fusión en Caliente/métodos , Polietilenglicoles/química , Humanos , Administración Bucal , Química Farmacéutica/métodos , Adipatos/química , Acrilatos/química , Ácidos Polimetacrílicos/química , Polímeros/química , Composición de Medicamentos/métodos
9.
Mar Pollut Bull ; 201: 116261, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38537567

RESUMEN

Marine microorganisms have been reported to degrade microplastics. However, the degradation mechanisms are still poorly understood. In this study, a bacterium Roseibium aggregatum ZY-1 was isolated from seawater, which can degrade poly(butylene adipate-co-terephthalate) (PBAT). The PBAT-PLA(polylactic acid, PLA) films, before and after degradation, were characterized by scanning electron microscope (SEM) and Fourier transform infrared spectrometer (FTIR), the weight loss rate and water contact angle were measured. The results indicate that ZY-1 colonized on PBAT-PLA film, changed the functional groups and decreased water contact angle of PBAT-PLA film. Moreover, liquid chromatography mass spectrometry (LC-MS) analysis reveales that PBAT was degraded into its oligomers (TB, BTB) and monomers (T, A) during 10 days, and adipic acid (A) could be used as a sole carbon source. The whole genome sequencing analyses illustrate the mechanisms and enzymes such as PETase, carboxylesterases, arylesterase (PpEst) and genes like pobA, pcaBCDFGHIJKT, dcaAEIJK, paaGHJ involved in PBAT degradation. Therefore, the R. aggregatum ZY-1 will be a promising candidate of PBAT degradation.


Asunto(s)
Alquenos , Ácidos Ftálicos , Plásticos , Poliésteres , Poliésteres/química , Adipatos/química , Bacterias/metabolismo , Agua
10.
J Control Release ; 369: 573-590, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38554773

RESUMEN

Postoperative abdominal adhesions are a common clinical problem after surgery and can cause many serious complications. Current most commonly used antiadhesion products are less effective due to their short residence time and focus primary on barrier function. Herein, we developed a sprayable hydrogel barrier (sHA-ADH/OHA-E) with self-regulated drug release based on ROS levels at the trauma site, to serve as a smart inflammatory microenvironment modulator and GATA6+ macrophages trap for non-adherent recovery from abdominal surgery. Sulfonated hyaluronic acid (HA) conjugates modified with adipic dihydrazide (sHA-ADH), and oxidized HA conjugates grafted with epigallocatechin-3-gallate (EGCG) via ROS-cleavable boronate bonds (OHA-E) were synthesized. sHA-ADH/OHA-E hydrogel was facilely fabricated within 5 s after simply mixing sHA-ADH and OHA-E through forming dynamic covalent acylhydrazones. With good biocompatibility, appropriate mechanical strength, tunable shear-thinning, self-healing, asymmetric adhesion, and reasonable in vivo retention time, sHA-ADH/OHA-E hydrogel meets the requirements of a perfect physical barrier. Intriguingly, sulfonic acid groups endowed the hydrogel with satisfactory anti-fibroblast and macrophage attachment capability, and were demonstrated for the first time to act as polyanion traps to prevent GATA6+ macrophages aggregation. Importantly, EGCG could be intelligently released by ROS triggering to alleviate oxidative stress and promote proinflammatory M1 macrophage polarize to antiinflammatory M2 phenotype. Further, the fibrinolytic system balance was restored to reduce fibrosis. Thanks to the above advantages, the sHA-ADH/OHA-E hydrogel exhibited excellent anti-adhesion effects in a rat sidewall defect-cecum abrasion model and is expected to be a promising and clinically translatable antiadhesion barrier.


Asunto(s)
Factor de Transcripción GATA6 , Ácido Hialurónico , Hidrogeles , Macrófagos , Complicaciones Posoperatorias , Especies Reactivas de Oxígeno , Adherencias Tisulares/prevención & control , Animales , Hidrogeles/química , Hidrogeles/administración & dosificación , Macrófagos/efectos de los fármacos , Macrófagos/metabolismo , Especies Reactivas de Oxígeno/metabolismo , Ácido Hialurónico/química , Complicaciones Posoperatorias/prevención & control , Factor de Transcripción GATA6/metabolismo , Catequina/análogos & derivados , Catequina/química , Catequina/administración & dosificación , Catequina/farmacología , Ratas Sprague-Dawley , Ratones , Adipatos/química , Masculino , Abdomen/cirugía , Células RAW 264.7 , Depuradores de Radicales Libres/administración & dosificación , Depuradores de Radicales Libres/química , Depuradores de Radicales Libres/farmacología , Liberación de Fármacos
11.
Int J Biol Macromol ; 259(Pt 2): 129355, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-38218295

RESUMEN

Polylactide/poly(butylene adipate-co-terephthalate) (PLA/PBAT) blends were compatibilized using dicumyl peroxide (DCP) and poly(ethylene glycol) 600 diacrylate (PEG600DA) through a one-step melt-blending process. The compatibility and performance of these blends were subsequently characterized. The results showed that grafts formed "in situ" effectively improved the compatibility and interfacial adhesion between PLA and PBAT phases. Melt viscosity and elasticity of both the PLA/PBAT/DCP and PLA/PBAT/DCP/PEG600DA blends evinced significant increases. Compared to PLA alone, both cold and melt crystallization abilities of the PLA/PBAT/DCP/PEG600DA blends were enhanced, with crystallinities increasing by 5 % - 10 %. Furthermore, the thermal stability, as well as hydrophobicity and oleophobicity of the compatibilized blends improved. In comparison with PLA, the elongation at break and notched impact strength for the PLA/PBAT/DCP/PEG600DA (60/40/0.1/4) blend achieved increases of 290 % and 44.23 kJ/m2, corresponding to improvements of 279 % and 1457 %, respectively. The toughening effect was substantially influenced by the ductile matrix (either a co-continuous phase or a flexible PBAT matrix) in addition to the strong interfacial adhesion and fine phase domain. These eco-friendly blends exhibit considerable potential for packaging articles and 3D printing products owing to their excellent mechanical properties and enhanced melt rheology.


Asunto(s)
Alquenos , Peróxidos , Ácidos Ftálicos , Poliésteres , Polietilenglicoles , Poliésteres/química , Adipatos/química
12.
Int J Biol Macromol ; 253(Pt 6): 127408, 2023 Dec 31.
Artículo en Inglés | MEDLINE | ID: mdl-37832616

RESUMEN

Food safety concerns from spoilage and non-degradable packaging risk human health. Progress made in biodegradable plastic films, but limited study on biomass composite films with favorable morphological, mechanical, and inherent antibacterial properties for fresh meat preservation. Herein, we present a versatile packaging film created through the extrusion blowing process, combining oxidized starch (OST) with poly(butylene adipate-co-terephthalate) (PBAT). SEM analysis revealed even distribution of spherical OST particles on film's surface. FTIR spectra revealed new intermolecular hydrogen bonds between OST and PBAT. While combining OST slightly reduced tensile properties, all composite films met the required strength of 16.5 ± 1.39 MPa. Notably, films with 40 % OST showed over 98 % antibacterial rate against Staphylococcus aureus within 2 h. pH wasn't the main cause of bacterial growth inhibition; OST hindered growth by interfering with nutrient absorption and metabolism due to its carboxyl groups. Additionally, OST disrupted bacterial membrane integrity and cytoplasmic membrane potential. Remarkably, the OST/PBAT film excellently preserved chilled fresh pork, maintaining TVB-N level at 12.6 mg/100 g on day 6, microbial count at 105 CFU/g within 6-10 days, and sensory properties for 8 days. It extended pork's shelf life by two days compared to polyethylene film, suggesting an alternative to a synthetic material.


Asunto(s)
Carne de Cerdo , Carne Roja , Humanos , Porcinos , Animales , Poliésteres/química , Almidón/química , Antibacterianos/farmacología , Antibacterianos/química , Embalaje de Alimentos , Adipatos/química
13.
Int J Biol Macromol ; 253(Pt 4): 126976, 2023 Dec 31.
Artículo en Inglés | MEDLINE | ID: mdl-37739283

RESUMEN

The poly(butylene adipate-co-terephthalate) (PBAT)/poly(lactic acid) (PLA) films have been widely used due to their biological degradability and excellent comprehensive properties. However, the reports regarding biodegradable PLA/PBAT films are rather scarce. In this work, systematical investigations of biaxially stretched PLA/PBAT films were performed. Compared with unstretched films, the PLA/PBAT 75/25 films with the stretching ratio of 5 × 1 exhibited an improvement on the crystallinity of PLA from 6 % to 58.6 %. According to 2D-WAXS results, the orientation of the α crystal in the MD increased with the increase of the stretching ratio. The stretched films showed favorable barrier properties. The oxygen permeability (OP) of 2 × 2 PLA/PBAT 75/25 films shows a decrement of 22 % compared with that of the unstretched films. Interestingly, the uniaxially stretched PLA/PBAT 75/25 films exhibits increased surface roughness (Ra) for 3 × 1 film whereas decreased Ra for the 5 × 1 film, which could be related to the phase separation under stretching. The tensile strength in the machine direction (MD) of the PLA/PBAT 75/25 films was improved up to 51.6 MPa for 5 × 1 film, which is 45 % higher than that of unstretched counterpart. The stretched films exhibit excellent mechanical and barrier properties, which could be utilized in packaging industry with high potential.


Asunto(s)
Oxígeno , Poliésteres , Oxígeno/química , Poliésteres/química , Embalaje de Alimentos/métodos , Adipatos/química
14.
Int J Biol Macromol ; 253(Pt 1): 126609, 2023 Dec 31.
Artículo en Inglés | MEDLINE | ID: mdl-37652334

RESUMEN

With increasing awareness on environmental protection and food safety, the development of biodegradable antimicrobial packaging materials has been paid growing emphasis. In this work, starch/poly(butylene adipate-co-terephthalate)/ε-polylysine hydrochloride films were prepared by extrusion blowing, and five commercial organically modified nanomontmorillonites (OMMT, including DK1, DK2, DK3, DK4, and DK5) were used as reinforcing agents. Intercalated structures were formed in the nanocomposite films, especially for those with DK3 and DK4 owing to their higher hydrophobicity and larger interlayer spacing. Adding OMMT weakened hydrogen bonds and the gelatinization/plasticization degree of starch. Morphology analysis revealed that the agglomeration of OMMT occurred in the films, but the film containing DK3 still showed a relatively homogeneous microstructure. Loading OMMT enhanced the strength, deformation resistance, thermal stability, surface hydrophobicity, but decreased barrier properties and water sensitivity of the films. Antimicrobial activity showed that the OMMT and ε-polylysine hydrochloride possessed a synergistic effect against Staphylococcus aureus and Escherichia coli. The maximum inhibition rate was observed in that with DK4, approaching 100 %. Findings supported the application of commercial OMMT in manufacturing biodegradable antimicrobial blown films.


Asunto(s)
Antiinfecciosos , Poliésteres , Poliésteres/química , Polilisina/química , Almidón/química , Antiinfecciosos/farmacología , Adipatos/química
15.
Bioresour Technol ; 385: 129430, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37399952

RESUMEN

PBAT (poly butylene adipate-co-terephthalate) is a widely used biodegradable plastic, but the knowledge about its metabolization in anaerobic environments is very limited. In this study, the anaerobic digester sludge from a municipal wastewater treatment plant was used as inoculum to investigate the biodegradability of PBAT monomers in thermophilic conditions. The research employs a combination of 13C-labelled monomers and proteogenomics to track the labelled carbon and identify the microorganisms involved. A total of 122 labelled peptides of interest were identified for adipic acid (AA) and 1,4-butanedio (BD). Through the time-dependent isotopic enrichment and isotopic profile distributions, Bacteroides, Ichthyobacterium, and Methanosarcina were proven to be directly involved in the metabolization of at least one monomer. This study provides a first insight into the identity and genomic potential of microorganisms responsible for biodegradability of PBAT monomers during anaerobic digestion under thermophilic conditions.


Asunto(s)
Carbono , Poliésteres , Poliésteres/metabolismo , Anaerobiosis , Adipatos/química
16.
Environ Res ; 235: 116634, 2023 10 15.
Artículo en Inglés | MEDLINE | ID: mdl-37442258

RESUMEN

The development of composites for food packaging that have good mechanical and antimicrobial characteristics is still a major challenge. In applications like food packaging, the usage of poly (butylene adipate-co-terephthalate) (PBAT), which has an adversative effect on the environment and reduces petroleum resources, has grown widespread. The present work reveals PBAT composites reinforced with CNPs at a few percentages up to 5.0 wt %. The PBAT/CNPs composites were produced using the solvent casting method. The results of TGA studies, CNPs significantly enhanced the thermal stability of composites using PBAT. The mechanical strength of the PBAT composites was improved by increasing CNPs concentration. Tensile strength increased from 7.38 to 10.22 MPa, respectively. The oxygen transmission rate (OTR) decreased with increasing the CNPs concentrations. The barrier properties (H2O and O2) of PBAT were improved by the presence of CNPs. WVTR was calculated to be 108.6 ± 1.8 g/m2/day for PBAT. WVTR reduced when CNPs concentration in PBAT increased. The PCN-5.0 film sample had the lowest WVTR value, 34.1 ± 3.1 g/m2/day. For PCN-3.0, WVTR dropped by 45.39%, indicating and even with a 3.0 wt% loading of CNPs in PBAT, the rise is noticeable. Contact angle measurements indicate that PBAT/CNPs composites becomes hydrophobic after reinforcing. Gram-positive (S. aureus) and Gram-negative (E. coli) food-borne pathogenic microorganisms showed enhanced antimicrobial activity against the developed PBAT composites. The carrot pieces preserved their freshness for an extended period of 12 days while packaged in the PBAT/CNPs composite film, indicating that the film is an effective and excellent packaging for food materials.


Asunto(s)
Nanopartículas , Poliésteres , Poliésteres/química , Escherichia coli , Staphylococcus aureus , Adipatos/química , Carbono
17.
Mar Pollut Bull ; 194(Pt B): 115295, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37517280

RESUMEN

Nylon fishing nets have excellent strength and durability, but when lost at sea, their insufficient decomposition destroys habitats and spawning grounds, and pollutes the marine environment. This led to the development of poly(butylene succinate) (PBS) resin for biodegradable fishing gear based on aliphatic fibers. Prompted by the low stiffness and elastic recovery of PBS, we introduced two additional components into the molecular structure of PBS: adipic acid and ethylene glycol. These two new components were combined with succinic acid and 1,4-butanediol, the existing components of PBS, to synthesize poly(butylene adipate-co-butylene succinate-co-ethylene adipate-co-ethylene succinate) (PBEAS) resin via esterification and polycondensation reactions of a quaternary aliphatic copolyester. Although the molecular weight and molecular weight distribution of PBEAS are similar to those of PBS, it has excellent tensile strength, stiffness, elastic recovery, and biodegradability, with a low melting point for good production efficiency. These improvements are expected to allow PBEAS resin to be applied to gill nets for fish that require high stiffness, thereby expanding the use of biodegradable fishing gear.


Asunto(s)
Poliésteres , Ácido Succínico , Animales , Poliésteres/química , Caza , Succinatos/química , Adipatos/química , Etilenos
18.
J Colloid Interface Sci ; 641: 1043-1057, 2023 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-36996683

RESUMEN

Sustainably derived poly(glycerol adipate) (PGA) has been deemed to deliver all the desirable features expected in a polymeric scaffold for drug-delivery, including biodegradability, biocompatibility, self-assembly into nanoparticles (NPs) and a functionalisable pendant group. Despite showing these advantages over commercial alkyl polyesters, PGA suffers from a series of key drawbacks caused by poor amphiphilic balance. This leads to weak drug-polymer interactions and subsequent low drug-loading in NPs, as well as low NPs stability. To overcome this, in the present work, we applied a more significant variation of the polyester backbone while maintaining mild and sustainable polymerisation conditions. We have investigated the effect of the variation of both hydrophilic and hydrophobic segments upon physical properties and drug interactions as well as self-assembly and NPs stability. For the first time we have replaced glycerol with the more hydrophilic diglycerol, as well as adjusting the final amphiphilic balance of the polyester repetitive units by incorporating the more hydrophobic 1,6-n-hexanediol (Hex). The properties of the novel poly(diglycerol adipate) (PDGA) variants have been compared against known polyglycerol-based polyesters. Interestingly, while the bare PDGA showed improved water solubility and diminished self-assembling ability, the Hex variation demonstrated enhanced features as a nanocarrier. In this regard, PDGAHex NPs were tested for their stability in different environments and for their ability to encode enhanced drug loading. Moreover, the novel materials have shown good biocompatibility in both in vitro and in vivo (whole organism) experiments.


Asunto(s)
Glicerol , Nanopartículas , Sistemas de Liberación de Medicamentos , Poliésteres/química , Preparaciones Farmacéuticas , Adipatos/química , Nanopartículas/química , Portadores de Fármacos/química
19.
J Hazard Mater ; 441: 129958, 2023 01 05.
Artículo en Inglés | MEDLINE | ID: mdl-36122523

RESUMEN

In recent years, Poly(butylene adipate-co-terephthalate) (PBAT) films were wildly used due to its biodegradable properties. However, there are few reports of strains that can high efficiently degrade PBAT. Thermobifida fusca FXJ-1, a thermophilic actinomycete, was screened and identified from compost. FXJ-1 can efficiently degrade PBAT at 55 °C in MSM medium. The degradation rates of the pure PBAT film (PF), PBAT film used for mulching on agricultural fields (PAF), and PBAT-PLA-ST film (PPSF) were 82.87 ± 1.01%, 87.83 ± 2.00% and 52.53 ± 0.54%, respectively, after nine days of incubation in MSM medium. Cracking areas were monitored uniformly distributed on the surfaces of three kinds of PBAT-based films after treatment with FXJ-1 using scanning electron microscopy. The LC-MS results showed that PBAT might be degraded into adipic acid, terephthalic acid, butylene adipate, butylene terephthalate and butylene adipate-co-terephthalate, and these products are involved in the cleavage of ester bonds. We also found that amylase produced by FXJ-1 played an important role in the degradation of PPSF. FXJ-1 also showed an efficient PBAT-based films degradation ability in simulating compost environment, which implied its potential application in PBAT and starch-based film degradation by industrial composting.


Asunto(s)
Compostaje , Poliésteres , Adipatos/química , Alquenos , Amilasas , Ésteres , Ácidos Ftálicos , Poliésteres/química , Almidón/química , Thermobifida
20.
Waste Manag ; 144: 1-10, 2022 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-35286847

RESUMEN

Poly(butylene adipate-co-terephthalate) (PBAT), a bioplastic consisting of aliphatic hydrocarbons and aromatic hydrocarbons, was developed to overcome the shortcomings of aliphatic and aromatic polyesters. Many studies report the use of PBAT as a blending material for improving properties of other bioplastics. However, there are few studies on microorganisms that degrade PBAT. We found six kinds of PBAT-degrading microorganisms from various soils. Among these, Bacillus sp. JY35 showed superior PBAT degradability and robustness to temperature. We monitored the degradation of PBAT films by Bacillus sp. JY35 using scanning electron microscopy, field emission scanning electron microscopy, Fourier-transform infrared spectroscopy, and gel permeation chromatography. GC-MS was used to measure the PBAT film degradation rate at different temperatures and with additional NaCl and carbon sources. Certain additional carbon sources improve the growth of Bacillus sp. JY35. However, this did not increase PBAT film degradation. Time-dependent PBAT film degradation rates were measured during three weeks of cultivation, after which the strain achieved almost 50% degradation. Additionally, various bioplastics were applied to solid cultures to confirm the biodegradation range of Bacillus sp. JY35, which can degrade not only PBAT but also PBS, PCL, PLA, PHB, P(3HB-co-4HB), P(3HB-co-3HV), P(3HB-co-3HHx), and P(3HB-co-3HV-co-3HHx), suggesting its usability as a superior bioplastic degrader.


Asunto(s)
Bacillus , Adipatos/química , Alquenos , Carbono , Ácidos Ftálicos , Poliésteres , Aguas del Alcantarillado , Aguas Residuales
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