Stability and release mechanism of double emulsification (W1/O/W2) for biodegradable pH-responsive polyhydroxybutyrate/cellulose acetate phthalate microbeads loaded with the water-soluble bioactive compound niacinamide.

Microbeads of biodegradable polyhydroxybutyrate (PHB) offer environmental benefits and economic competitiveness. The aim of this study was to encapsulate a water-soluble bioactive compound, niacinamide (NIA), in a pH-responsive natural matrix composed of PHB and cellulose acetate phthalate (CAP) by double emulsification (W1/O/W2) to improve the encapsulation efficiency (%EE) and loading capacity (%LC). PHB was produced in-house by Escherichia coli JM109 pUC19-23119phaCABA-04 without the inducing agent isopropyl ß-D-1-thiogalactopyranoside (IPTG). The influences of PHB and polyvinyl alcohol (PVA) concentrations, stirring rate, PHB/CAP ratio and initial NIA concentration on the properties of NIA-loaded pH-responsive microbeads were studied. The NIA-loaded pH-responsive PHB/CAP microbeads exhibited a spherical core-shell structure. The average size of the NIA-loaded pH-responsive microbeads was 1243.3 ± 11.5 µm. The EE and LC were 33.3 ± 0.5 % and 28.5 ± 0.4 %, respectively. The release profiles of NIA showed pH-responsive properties, as 94.2 ± 3.5 % of NIA was released at pH 5.5, whereas 99.3 ± 2.4 % of NIA was released at pH 7.0. The NIA-loaded pH-responsive PHB/CAP microbeads were stable for >90 days at 4 °C under darkness, with NIA remaining at 73.65 ± 1.86 %. A cytotoxicity assay in PSVK1 cells confirmed that the NIA-loaded pH-responsive PHB/CAP microbeads were nontoxic at concentrations lower than 31.3 µg/mL, in accordance with ISO 10993-5.

Fabrication, characterization and release behavior of α-tocopherol acetate-loaded pH-responsive polyhydroxybutyrate/cellulose acetate phthalate microbeads.

Microbeads are used in personal care and cosmetic products (PCCPs) but are produced from nondegradable materials. Biodegradable polyhydroxybutyrate (PHB) has been recognized as a promising alternative material for use in PCCPs; however, utilizing PHB to encapsulate PCCPs is challenging because PCCPs need to be protected from the environment but their release needs to be permitted under specific physiological conditions. The aim of this work was to develop and evaluate pH-responsive cellulose acetate phthalate (CAP) to formulate lipophilic α-tocopherol acetate (α-TA)-loaded pH-responsive PHB/CAP microbeads. The influences of the PHB/CAP ratio and initial α-TA loading on the microbead size, surface morphology, encapsulation efficiency (%EE), loading capacity (%LC), and α-TA release profile were studied. The microbeads exhibited a spherical shape with a size of 328.7 ± 2.9 µm. The EE and LC were 86.7 ± 2.6 % and 13.5 ± 0.4 %, respectively. The release profile exhibited pH-responsive characteristics. These α-TA-loaded pH-responsive microbeads were stable with >50 % of the α-TA remaining after 90 days at 4, 25 and 45 °C in the dark. The results from the cytotoxicity assay with PSVK1 cells demonstrated that the microbeads were nontoxic. Hence, our developed formulation has the potential to be used to encapsulate oil-based drugs to formulate lipophilic substance-loaded pH-responsive microbeads.

Preparation and characterization of astaxanthin-loaded biodegradable polyhydroxybutyrate (PHB) microbeads for personal care and cosmetic applications.

Due to its biodegradability and biocompatibility, polyhydroxybutyrate (PHB) has received attention as an alternative material for microbeads in personal care and cosmetic products (PCCPs). Here, PHB was produced from crude glycerol by an Escherichia coli JM109 strain harboring pUC19-23,119-phaCABA-04 without isopropyl ß-D-1-thiogalactopyranoside (IPTG), an inducing agent. Astaxanthin-loaded PHB microbeads were prepared through emulsification-solvent evaporation. Studies were performed to determine how the concentration of PHB and stirring rate influence the size, surface morphology, encapsulation efficiency (EE), and astaxanthin release profile. The astaxanthin-loaded PHB microbeads exhibited a rough surface, 98.1 ± 0.7 % EE, spherical shape and 179 ± 44 µm size. In addition, <50 % astaxanthin release was observed within 240 min. Stability studies revealed that astaxanthin-loaded microbeads retained over 85.3 ± 4.2 % of astaxanthin after 90 days at 4 °C and showed a 2-fold reduction in astaxanthin degradation compared to their unencapsulated counterparts; thus, astaxanthin-loaded microbeads show promise for PCCPs applications. A cytotoxicity assay revealed that astaxanthin-loaded PHB microbeads were nontoxic to the human epidermal keratinocyte cell line, PSVK1, and EpiSkin® cells. Skin irritation and sensitization were not observed during a human repeated insult patch test (HRIPT), according to clinical practice guidelines of the Japanese dermatological association.

Valorization of agro-industrial waste from the cassava industry as esterified cellulose butyrate for polyhydroxybutyrate-based biocomposites.

The aim of this study was to utilize cassava pulp to prepare biocomposites comprising microcrystalline cellulose from cassava pulp (CP-MCC) as a filler and polyhydroxybutyrate (PHB) synthesized in-house by Cupriavidus necator strain A-04. The CP-MCC was extracted from fresh cassava pulp. Next, the CP-MCC surface was modified with butyryl chloride (esterified to CP-MCC butyrate) to improve dissolution and compatibility with the PHB. FTIR results confirmed that the esterified CP-MCC butyrate had aliphatic chains replacing the hydroxyl groups; this substitution increased the solubilities in acetone, chloroform, and tetrahydrofuran. Biocomposite films were prepared by varying the composition of esterified CP-MCC butyrate as a filler in the PHB matrix at 0, 5, 10, 15, 20 and 100 wt%. The results for the 95:5 and 90:10 CP-MCC butyrate biocomposite films showed that esterification led to improvements in the thermal properties and increased tensile strengths and elongations at break. All prepared biocomposite films maintained full biodegradability.

Green composites made of polyhydroxybutyrate and long-chain fatty acid esterified microcrystalline cellulose from pineapple leaf.

Pineapple leaf fibres are an abundant agricultural waste product that contains 26.9% cellulose. The objective of this study was to prepare fully degradable green biocomposites made of polyhydroxybutyrate (PHB) and microcrystalline cellulose from pineapple leaf fibres (PALF-MCC). To improve compatibility with PHB, the PALF-MCC was surface modified using lauroyl chloride as an esterifying agent. The influence of the esterified PALF-MCC laurate content and changes in the film surface morphology on biocomposite properties was studied. The thermal properties obtained by differential scanning calorimetry revealed a decrease in crystallinity for all biocomposites, with 100 wt% PHB displaying the highest values, whereas 100 wt% esterified PALF-MCC laurate showed no crystallinity. The addition of esterified PALF-MCC laurate increased the degradation temperature. The maximum tensile strength and elongation at break were exhibited when adding 5% of PALF-MCC. The results demonstrated that adding esterified PALF-MCC laurate as a filler in the biocomposite film could retain a pleasant value of tensile strength and elastic modulus whereas a slight increase in elongation can help to enhance flexibility. For soil burial testing, PHB/ esterified PALF-MCC laurate films with 5-20% (w/w) PALF-MCC laurate ester had higher degradation than films consisting of 100% PHB or 100% esterified PALF-MCC laurate. PHB and esterified PALF-MCC laurate derived from pineapple agricultural wastes are particularly suitable for the production of relatively low-cost biocomposite films that are 100% compostable in soil.

Toughening and thermal characteristics of plasticized polylactide and poly(butylene adipate-co-terephthalate) blend films: Influence of compatibilization.

Bio-based polylactide (PLA) derived from fermented corn starch was blended with poly(butylene adipate-co-terephthalate) (PBAT) and triethyl citrate (TEC) plasticizer using a twin screw extruder. PLA-grafted-maleic anhydride (PLA-g-MA) synthesized via reactive maleation and toluene diisocyanate (TDI) were used as compatibilizers for these blends. Improvements in the toughness, phase morphology and thermal behavior of the PLA/PBAT/TEC (PBT) blend films were evaluated in terms of compatibilization effect. The compatibilized PBT blends showed noticeably superior tensile strength, elongation, and tensile-impact toughness compared with uncompatibilized ones due to the greater compatibility of PLA and PBAT phases. Well dispersed PBAT particles and many elongated fibrils were observed on the fracture surface of the film after compatibilization. Both TDI and PLA-g-MA were effective compatibilizers for the blend at an appropriate level. The addition of PLA-g-MA to the plasticized blends not only significantly enhanced mechanical properties and phase adhesion, but also accelerated cold crystallization and formed crystal perfection, a result of improvements in chain mobility and packing efficiency. Differential scanning calorimetry (DSC) results revealed changes in Tg and melting behavior of the blends from influences of compatibilization. The different types and levels of compatibilizer affected the thermal stability of the PLA phase but did not affect char remaining.

Facile isolation of cellulose nanofibers from water hyacinth using water-based mechanical defibrillation: Insights into morphological, physical, and rheological properties.

The utilization from biomass feedstocks to fabricate the advanced nanomaterials has greatly attracted a great interest due to their low cost and sustainability. This work aimed to explore a simple way to prepare cellulose nanofibers using water-based approach via mechanical defibrillation. Cellulose fibers were first extracted from water hyacinth towards chemical treatments and then mechanically disintegrated as a function of defibrillation cycles. The morphologies, thermal stabilities, physical properties, and rheological characteristics of the micro- and nanofibers were demonstrated. It was found that the obtained nanofibers having a diameter of 5-50 nm and were successfully prepared within 10 defibrillation cycles. Even though longer defibrillation cycles greatly provided higher water retention value and specific surface area, a gradual decrease in crystallinity index, thermal degradation temperatures, and degree of polymerization was also observed. Based on the rheological properties, the storage modulus and steady viscosity of the as-prepared nanofibers suspension increased significantly as a function of defibrillation, resulting in a gel-like structure with a shear-thinning behavior. Additionally, the rheological parameters of the obtained nanofibers estimated using a Herschel-Bulkley model were more accurate than that estimated using a Bingham-Plastic model. The obtained nanofibers could be used as a prime candidate for many potential applications.

Development and application of nanofibrillated cellulose coating for shelf life extension of fresh-cut vegetable during postharvest storage.

Food loss is a global concern nowadays. Fresh produce has the highest rate of loss among food products. In this study, nanocellulose suspensions were employed to coat on a perishable vegetable (spinach) for extending its shelf life during postharvest storage. Two mechanical defibrillation methods were studied to obtain a suitable preparation of nanocellulose suspension. A method of stock gel dilutions was selected since it provided longer stability of nanocellulose suspension. Then, physiological changes of spinach leaves coated with nanocellulose were measured compared with uncoated leaves. The results revealed that the coated leaves with 0.3 and 0.5% w/v nanocellulose concentrations displayed the significant retentions of appearance, chlorophyll, color, and moisture content after 3-day storage at 25 °C. Moreover, all of the coated samples exhibited the significant reduction of respiration rate in the range of 54-70%. These finding suggested that the nanocellulose coating improves the storage capacity of spinach.

Cellulose esters from waste cotton fabric via conventional and microwave heating.

The esterification of cellulose from waste cotton fabric in a N,N-dimethylacetamide/lithium chloride solvent system was carried out using different types of fatty acid chloride including butyryl chloride, capryloyl chloride, and lauroyl chloride as esterifying agents, and N,N-dimethyl 1-4-aminopyridine as a catalyst under conventional and microwave activation. Microwave esterification was performed under 2.45GHz with power varying from 90 to 450W. The optimum conditions for esterification of cotton cellulose with various esterifying agents were investigated in terms of reaction time and temperature to attain appropriate %weight increase and degree of substitution of esterified-cellulose. The degree of substitution, functional group and chemical structure, and thermal stability of cellulose ester powder were characterized by 1H NMR, FTIR, and TGA/SDTA analysis. Morphologies, crystallinity, and solubility of modified cellulose by two different heating methods were compared.