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1.
World J Microbiol Biotechnol ; 40(6): 172, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38630153

RESUMO

The exploitation of exciting features of plastics for diverse applications has resulted in significant plastic waste generation, which negatively impacts environmental compartments, metabolic processes, and the well-being of aquatic ecosystems biota. A shotgun metagenomic approach was deployed to investigate the microbial consortia, degradation pathways, and enzyme systems involved in the degradation of plastics in a tropical lentic pond sediment (APS). Functional annotation of the APS proteome (ORFs) using the PlasticDB database revealed annotation of 1015 proteins of enzymes such as depolymerase, esterase, lipase, hydrolase, nitrobenzylesterase, chitinase, carboxylesterase, polyesterase, oxidoreductase, polyamidase, PETase, MHETase, laccase, alkane monooxygenase, among others involved in the depolymerization of the plastic polymers. It also revealed that polyethylene glycol (PEG), polyhydroxyalkanoates (PHA), polyhydroxybutyrate (PHB), polylactic acid (PLA), polybutylene adipate terephthalate (PBAT), polyethylene terephthalate (PET), and nylon have the highest number of annotated enzymes. Further annotation using the KEGG GhostKOALA revealed that except for terephthalate, all the other degradation products of the plastic polymers depolymerization such as glyoxylate, adipate, succinate, 1,4-butanediol, ethylene glycol, lactate, and acetaldehyde were further metabolized to intermediates of the tricarboxylic acid cycle. Taxonomic characterization of the annotated proteins using the AAI Profiler and BLASTP revealed that Pseudomonadota members dominate most plastic types, followed by Actinomycetota and Acidobacteriota. The study reveals novel plastic degraders from diverse phyla hitherto not reported to be involved in plastic degradation. This suggests that plastic pollution in aquatic environments is prevalent with well-adapted degrading communities and could be the silver lining in mitigating the impacts of plastic pollution in aquatic environments.


Assuntos
Ecossistema , Consórcios Microbianos , Ácidos Ftálicos , Consórcios Microbianos/genética , Lagoas , Lipase , Adipatos , Polímeros
2.
Colloids Surf B Biointerfaces ; 236: 113828, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38452625

RESUMO

Despite the success of polyethylene glycol-based (PEGylated) polyesters in the drug delivery and biomedical fields, concerns have arisen regarding PEG's immunogenicity and limited biodegradability. In addition, inherent limitations, including limited chemical handles as well as highly hydrophobic nature, can restrict their effectiveness in physiological conditions of the polyester counterpart. To address these matters, an increasing amount of research has been focused towards identifying alternatives to PEG. One promising strategy involves the use of bio-derived polyols, such as glycerol. In particular, glycerol is a hydrophilic, non-toxic, untapped waste resource and as other polyols, can be incorporated into polyesters via enzymatic catalysis routes. In the present study, a systematic screening is conducted focusing on the incorporation of 1,6-hexanediol (Hex) (hydrophobic diol) into both poly(glycerol adipate) (PGA) and poly(diglycerol adipate) (PDGA) at different (di)glycerol:hex ratios (30:70; 50:50 and 70:30 mol/mol) and its effect on purification upon NPs formation. By varying the amphiphilicity of the backbone, we demonstrated that minor adjustments influence the NPs formation, NPs stability, drug encapsulation, and degradation of these polymers, despite the high chemical similarity. Moreover, the best performing materials have shown good biocompatibility in both in vitro and in vivo (whole organism) tests. As preliminary result, the sample containing diglycerol and Hex in a 70:30 ratio, named as PDGA-Hex 30%, has shown to be the most promising candidate in this small library analysed. It demonstrated comparable stability to the glycerol-based samples in various media but exhibited superior encapsulation efficiency of a model hydrophobic dye. This in-depth investigation provides new insights into the design and modification of biodegradable (di)glycerol-based polyesters, potentially paving the way for more effective and sustainable PEG-free drug delivery nano-systems in the pharmaceutical and biomedical fields.


Assuntos
Nanopartículas , Poliésteres , Poliésteres/química , Glicerol/química , Polietilenoglicóis/química , Sistemas de Liberação de Medicamentos , Preparações Farmacêuticas , Adipatos , Nanopartículas/química
3.
Mar Pollut Bull ; 201: 116261, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38537567

RESUMO

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.


Assuntos
Alcenos , Ácidos Ftálicos , Plásticos , Poliésteres , Poliésteres/química , Adipatos/química , Bactérias/metabolismo , Água
4.
J Mech Behav Biomed Mater ; 153: 106493, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38484428

RESUMO

Elastomeric biocomposites based on poly(glycerol adipate urethane) and hydroxyapatite were fabricated for tissue regeneration. The poly(glycerol adipate urethane) (PGAU) elastomeric composite matrices were obtained by chemical crosslinking of the poly(glycerol adipate) prepolymer (pPGA) with diisocyanate derivative of L-lysine. Two series of composites varying in the amount of L-lysine diisocyanate ethyl ester (LDI) used as a crosslinking agent were manufactured. As a ceramic filler both unmodified and L-lysine surface-modified hydroxyapatite (HAP) particles were used. The novelty of our research consists in the manufactured elastomeric materials and characterization of their linear viscoelastic (LVE) properties. The LVE properties of the composites were investigated by means of dynamic thermomechanical analysis. Frequency sweep and amplitude sweep measurements were performed in shear mode. The influence of the crosslinking agent (LDI) amount, HAP content and surface modification of HAP on the LVE properties of the composites was determined based on the analysis of the master curves of storage (G') and loss (G″) moduli and of tanδ of the composites. Depending on the amount of LDI, HAP and surface modification, the materials differ in the values of rubber elasticity plateau modulus (G0) and G' and G″ determined at selected shear frequencies and at the glassy state. G0 ranges from 278 kPa to 3.98 MPa, G' in the glassy state is within the range of 219 MPa-459 MPa. The G0 values of the PGAU-based composites are within the stiffness range of soft tissue. In view of the choice of HAP as the ceramic component and the G0 values, elastomeric composites have the potential to be used as filling materials in small bone defects (due to their mechanical similarity to osteoid) as well as materials for cartilage tissue regeneration.


Assuntos
Glicerol , Uretana , Glicerol/química , Lisina/química , Teste de Materiais , Elasticidade , Durapatita/química , Adipatos , Ésteres
5.
Chemosphere ; 353: 141554, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38430940

RESUMO

Microbial biodegradation of commercially available poly(butylene adipate-co-terephthalate)-polylactic acid-thermoplastic starch based bio-plastic has been pursued at high temperatures exceeding 55 °C. Herein, we first reported three newly isolated fungal strains from farmland soil samples of Republic of Korea namely, Pyrenochaetopsis sp. strain K2, Staphylotrichum sp. S2-1, and Humicola sp. strain S2-3 were capable of degrading a commercial bio-plastic film with degradation rates of 9.5, 8.6, and 12.2%, respectively after 3 months incubation at ambient conditions. Scanning electron microscopy (SEM) analyses showed that bio-plastic film was extensively fragmented with severe cracking on the surface structure after incubation with isolated fungal strains. X-ray diffraction (XRD) analysis also revealed that high crystallinity of the commercial bio-plastic film was significantly decreased after degradation by fungal strains. Liquid chromatography-mass spectrometry (LC-MS) analyses of the fungal culture supernatants containing the bio-plastic film showed the peaks for adipic acid, terephthalic acid (TPA), and terephthalate-butylene (TB) as major metabolites, suggesting cleavage of ester bonds and accumulation of TPA. Furthermore, a consortium of fungal strain K2 with TPA degrading bacterium Pigmentiphaga sp. strain P3-2 isolated from the same sampling site exhibited faster degradation rate of the bio-plastic film within 1 month of incubation with achieving complete biodegradation of accumulated TPA. We assume that the extracellular lipase activity presented in the fungal cultures could hydrolyze the ester bonds of PBAT component of bio-plastic film. Taken together, the fungal and bacterial consortium investigated herein could be beneficial for efficient biodegradation of the commercial bio-plastic film at ambient conditions.


Assuntos
Alcenos , Ácidos Ftálicos , Poliésteres , Amido , Amido/química , Poliésteres/química , Adipatos , Fungos , Ésteres
6.
Int J Biol Macromol ; 265(Pt 1): 130834, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38484815

RESUMO

Blending poly (butylene adipate-co-terephthalate) (PBAT) and polylactic acid (PLA) is a cost-effective strategy to obtain biodegradable plastic with complementary properties. However, the incompatibility between PBAT and PLA is a great challenge for fabricating high-performance composite films. Herein, the ethyl acetate fractionated lignin with the small glass transition temperature and low molecular weight was achieved and incorporated into the PBAT/PLA composite as a compatibilizer. The fractionated lignin can be uniformly dispersed within the PBAT/PLA matrix through a melt blending process and interact with the molecular chain of PBAT and PLA as a bonding bridge, which enhances the intermolecular interactions and reduces the interfacial tension of PBAT/PLA. By adding fractionated lignin, the tensile strength of the PBAT/PLA composite increased by 35.4 % and the yield strength increased by 37.7 %. Owing to lignin, the composite films possessed the ultraviolet shielding function and exhibited better water vapor barrier properties (1.73 ± 0.08 × 10-13 g·cm/cm2·s·Pa). This work conclusively demonstrated that fractionated lignin can be used as a green compatibilizer and a low-cost functional filler for PBAT/PLA materials, and provides guidance for the application of lignin in biodegradable plastics.


Assuntos
Alcenos , Plásticos Biodegradáveis , Lignina , Ácidos Ftálicos , Adipatos , Poli A , Poliésteres
7.
Int J Biol Macromol ; 263(Pt 2): 130147, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38354942

RESUMO

Green polymeric foams are an important research topic for sustainable development. In this study, a natural multifunctional flame-retardant additive based on food waste was developed and evaluated for its ability to replace the commercial additives tricresyl phosphate (TCP) and trioctyl phosphate (TOP) in a polylactide/poly(butylene adipate-co-terephthalate) (PLA/PBAT) foam. A series of blend foams with additives were prepared by melt extrusion. According to the results, the blend foam with 20 phr of TCP showed the best combination of impact toughness and flame retardancy. TCP, however, poses health and environmental risks. Therefore, natural flame retardants (NFRs) were used to partially replace the commercial flame retardant (CFR). A combination of TCP and soybean residue (SB) produced an impact toughened and flame-retardant blend foam. When compared to the neat PLA/PBAT foam, the impact toughness of the best sample was increased by about 256 %. The optimal foam showed excellent flame resistance with a V-0 UL-94 rating and a high LOI value (31.8 %). SB has the potential to partially replace TCP as flame retardant and could be used in a broad range of PLA/PBAT foam applications.


Assuntos
Alcenos , Retardadores de Chama , Ácidos Ftálicos , Eliminação de Resíduos , Fósforo , 60659 , Alimentos , Poliésteres , Adipatos , Poli A
8.
J Hazard Mater ; 467: 133680, 2024 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-38325094

RESUMO

Biodegradable mulches are widely recognized as ecologically friendly substances. However, their degradation percentage upon entering soils may vary based on mulch type and soil microbial activities, raising concerns about potential increases in microplastics (MPs). The effects of using different types of mulch on soil carbon pools and its potential to accelerate their depletion have not yet well understood. Therefore, we conducted an 18-month experiment to investigate mulch biodegradation and its effects on CO2 emissions. The experiment included burying soil with biodegradable mulch made of polylactic acid (PLA) and polybutylene adipate terephthalate (PBAT), and control treatments with traditional mulch (PE) and no mulch (CK). The results indicated that PE did not degrade, and the degradation percentage of PLA and PBAT were 46.2% and 88.1%, and the MPs produced by the degradation were 6.7 × 104 and 37.2 × 104 items/m2, respectively. Biodegradable mulch, particularly PLA, can enhance soil microbial diversity and foster more intricate bacterial communities compared to PE. The CO2 emissions were 0.58, 0.74, 0.99, and 0.86 g C/kg in CK, PE, PLA, , PBAT, respectively. A positive correlation was observed between microbial abundance and diversity with CO2 emissions, while a negative correlation was observed with soil total organic carbon. Biodegradable mulch enhanced the transformation of soil organic C into CO2 by stimulating microbial activity.


Assuntos
Adipatos , Dióxido de Carbono , Microplásticos , Microplásticos/toxicidade , Plásticos , Carbono , Poliésteres , Solo
9.
Int J Biol Macromol ; 262(Pt 1): 129880, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38307427

RESUMO

The preparation and characterization of lignin nanoparticles (LNPs) were described. LNPs were produced via the precipitation technique. Nanocomposites of LNPs with poly (butylene adipate-co-terephthalate) (PBAT) were prepared by melt mixing with various concentrations up to 6 wt% of LNPs. The assessment of the effects of LNP addition on the mechanical, thermal, morphological, cytotoxicity, antioxidant, antibacterial, and antiviral properties of nanocomposites was carefully performed. The addition of LNPs to PBAT enhances the thermal stability of the nanocomposites. The antioxidant effect of LNPs on PBAT increased with increasing filler content. LNPs showed higher efficiency as antioxidant agents than lignin particles (LP). The tensile modulus increased by 20 % for the nanocomposites with 6 % LNPs in comparison with neat PBAT. The crystallization peak temperature of PBAT was 80 °C, which increased to 104.6 °C with the addition of 6 wt% of LNPs, suggesting their strong nucleation activity. Antibacterial tests demonstrated the bacteriostatic activities of LNP, LP, and nanocomposites. Both LP and LNP showed considerable antiviral activity against herpes simplex virus type 1 and human coronavirus 229e. The antiviral activity of LNP was concentration-dependent. The findings suggest that LNP is a promising bio-additive for PBAT and can enhance its properties for various applications, including food packaging.


Assuntos
Alcenos , Nanopartículas , Ácidos Ftálicos , Poliésteres , Humanos , Poliésteres/química , Lignina/farmacologia , Antioxidantes/farmacologia , Antibacterianos/farmacologia , Adipatos , Nanopartículas/química , Antivirais/farmacologia
10.
Int J Biol Macromol ; 262(Pt 1): 129998, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38336326

RESUMO

How to effectively improve the poor interfacial adhesion between polylactic acid/poly(butylene adipate-co-terephthalate) (PLA/PBAT) matrix and thermoplastic starch (TPS) is still a challenge. Therefore, this work aims to introduce a convenient method to enhance the performance of PLA/PBAT/TPS blend by melt reactive extrusion. Here, using 4,4'-methylene-bis(N,N-diglycidyl-aniline) (MBDG) containing four epoxy groups as a reactive compatibilizer, and respectively using 1-methylimidazole (MI) or triethylenediamine (TD) as a catalyzer, serial PLA/PBAT/TPS ternary bio-composites are successfully prepared via melt reactive extrusion. The results showed that, under the catalysis of organic base, especially MI, the epoxy groups of MBDG can effectively react with hydroxyl and carboxyl groups of PLA/PBAT and hydroxyl groups in TPS to form chain-expanded and cross-linked structures. The tensile strength of the composites is increased by 20.0 % from 21.1 MPa, and the elongation at break is increased by 182.4 % from 17.6 % owing to the chain extension and the forming of cross-linked structures. The molecular weight, thermal stability, crystallinity, and surface hydrophobicity of the materials are gradually improved with the increase of MBDG content. The melt fluidity of the composites is also improved due to the enhancement of compatibility. The obtained PLA/PBAT/TPS materials have the potential to be green plastic products with good properties.


Assuntos
Alcenos , Resinas Epóxi , Ácidos Ftálicos , Poliésteres , Adipatos , Amido
11.
Int J Biol Macromol ; 262(Pt 1): 130029, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38340935

RESUMO

The wide application of fully biodegradable polylactic acid/polybutylene terephthalate (PLA/PBAT) blends in environmentally friendly packaging were limited because of poor compatibility. Normal compatibilizers suffer from poor thermal stability and non-biodegradability. In this work, epoxy copolymer (MDOG) with different molecular structures were made of 2-methylene-1, 3-dioxoheptane, and glycidyl methacrylate as raw materials by free radical copolymerization. MDOG copolymers have good biodegradability and a high thermal decomposition temperature of 361 °C. The chemical reaction of the epoxy groups in MDOG with PLA and PBAT during the melting reaction improved the interfacial bonding by decreasing the particle size of PBAT. Compared to the PLA/PBAT blends, the tensile strength and fracture toughness of PLA/PBAT/MDOG blends were enhanced to 34.6 MPa and 115.8 MJ/m3, which are 25 % and 81 % higher, respectively. As a result, this work offers new methods for developing thermally stable and biodegradable compatibilizers, which will hopefully promote the development of packaging industry.


Assuntos
Adipatos , Alcenos , Ácidos Ftálicos , Poliésteres , Polímeros , Resinas Epóxi , Poli A , Ácido Láctico
12.
Int J Biol Macromol ; 263(Pt 1): 130232, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38373561

RESUMO

Active packaging relies on controlled release of antimicrobials for food protection; however, uncontrolled migration due to environmental factors poses safety and functionality challenges. This study investigated the stability of zinc oxide nanoparticle (ZnONP) in poly(butylene-adipate-co-terephthalate)/thermoplastic starch (PBAT/TPS) biopolymer film for active food packaging applications. While incorporating ZnONP significantly enhanced the properties and active functionalities (UV-light blocking, antimicrobial activity) of PBAT/TPS film, food simulants posed significant stability challenges. Notably, exposure to 3 % acetic acid (acidic food simulant) triggered complete detachment and dissolution of ZnONPs from the film surface, leading to pore formation and subsequent internal ZnO dissolution. This resulted in dramatic alterations to the bionanocomposite films, including increased opacity, water vapor permeability, and decreased thermal stability, mechanical properties, and active functionalities. In contrast, 10 % ethanol (aqueous food simulant) had minimal impact, suggesting higher ZnO stability in neutral environments. Importantly, ZnO migration analysis revealed thresholds for safe application: 1 % ZnONP for acidic food contact and up to 5 % for aqueous foodstuffs. These findings highlight the critical role of environmental factors in ZnONP stability and emphasize the need for strategic optimization of ZnO content for achieving both functionality and safety in active biopolymer packaging.


Assuntos
Ácidos Ftálicos , Polienos , Óxido de Zinco , Amido , Poliésteres , Adipatos
13.
Microbiol Spectr ; 12(3): e0381923, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38305171

RESUMO

Gut microbiota plays a vital role in obtaining nutrition from bamboo for giant pandas. However, low cellulase activity has been observed in the panda's gut. Besides, no specific pathway has been implicated in lignin digestion by gut microbiota of pandas. Therefore, the mechanism by which they obtain nutrients is still controversial. It is necessary to elucidate the precise pathways employed by gut microbiota of pandas to degrade lignin. Here, the metabolic pathways for lignin degradation in pandas were explored by comparing 209 metagenomic sequencing data from wild species with different feeding habits. Lignin degradation central pathways, including beta-ketoadipate and homogentisate pathway, were enriched in the gut of wild bamboo-eating pandas. The gut microbiome of wild bamboo-eating specialists was enriched with genes from pathways implicated in degrading ferulate and p-coumarate into acetyl-CoA and succinyl-CoA, which can potentially provide the raw materials for metabolism in pandas. Specifically, Pseudomonas, as the most dominant gut bacteria genus, was found to be the main bacteria to provide genes involved in lignin or lignin derivative degradation. Herein, three Pseudomonas-associated strains isolated from the feces of wild pandas showed the laccase, lignin peroxidase, and manganese peroxidase activity and extracellular lignin degradation ability in vitro. A potential mechanism for pandas to obtain nutrition from bamboo was proposed based on the results. This study provides novel insights into the adaptive evolution of pandas from the perspective of lignin metabolism. IMPORTANCE: Although giant pandas only feed on bamboo, the mechanism of lignin digestion in pandas is unclear. Here, the metabolic pathways for lignin degradation in wild pandas were explored by comparing gut metagenomic from species with different feeding habits. Results showed that lignin degradation central pathways, including beta-ketoadipate and homogentisate pathway, were enriched in the gut of wild bamboo-eating pandas. Genes from pathways involved in degrading ferulate and p-coumarate via beta-ketoadipate pathway were also enriched in bamboo-eating pandas. The final products of the above process, such as acetyl-CoA, can potentially provide the raw materials for metabolism in pandas. Specifically, Pseudomonas, as the most dominant gut bacteria genus, mainly provides genes involved in lignin degradation. Herein, Pseudomonas-associated strains isolated from the feces of pandas could degrade extracellular lignin. These findings suggest that gut microbiome of pandas is crucial in obtaining nutrition from lignin via Pseudomonas, as the main lignin-degrading bacteria.


Assuntos
Adipatos , Lignina , Ursidae , Animais , Lignina/metabolismo , Ursidae/metabolismo , Ursidae/microbiologia , Acetilcoenzima A , Pseudomonas/genética , Pseudomonas/metabolismo , Bactérias
14.
Anal Methods ; 16(11): 1579-1592, 2024 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-38407576

RESUMO

Phthalates or phthalic acid esters (PAE) and bis(2-ethylhexyl)adipate (DEHA) are ubiquitous chemicals often used as plasticisers and additives in many industrial products and are classified as both persistent organic pollutants (POPs) and new emerging pollutants (NEPs). Exposure to these chemicals, especially through inhalation, is linked to a wide range of negative health effects, including endocrine disruption. Air particulate matter (PM) with an aerodynamic diameter ≤ 2.5 µm can be enriched with PAEs and DEHA and if inhaled can cause multi-system human toxicity. Therefore, proper monitoring of PAEs and DEHA in PM is required to assess human exposure to these pollutants. In this work, we developed and validated a new and sensitive gas-chromatography high-resolution mass spectrometry (GC-HRMS) method for targeted analysis of PAEs including dimethyl phthalate (DMP), diethyl phthalate (DEP), di-n-butyl phthalate (DBP), benzyl butyl phthalate (BBP), bis(2-ethylhexyl)adipate (DEHA), bis(2-ethylhexyl)phthalate (DEHP), di-n-octyl phthalate (DOP), in PM. Analytical aspects including sample preparation steps and GC-HRMS parameters, e.g., quadrupole isolation window, to enhance method sensitivity have been assessed. The estimated limit of detection (LODs) of target PAEs and DEHA ranged from 5.5 to 17 pg µL-1, allowing their trace-level detection in PM. Extraction efficiencies of 78-101% were obtained for the target compounds. Low DMP and DEP extraction efficiencies from the spiked filter substrates indicated that significant losses of higher volatility PAEs can occur during the sample collection when filter-based techniques are used. This work is the first targeted method based on GC-Orbitrap MS for PAEs and DEHA in environmental samples. The validated method was successfully applied for the targeted analysis of PAEs and DEHA in PM2.5 samples from the eighth most populous city in Brazil, Curitiba. This work is the first to report DBP, DEHA, DEHP, and DOP in urban PM from Brazil. The observed concentrations of PAEs (up to 29 ng m-3) in PM2.5 from Curitiba may not represent the extent of pollution by these toxic compounds since the analysed samples were collected during a COVID-19 restriction when anthropogenic activities were reduced.


Assuntos
Dietilexilftalato , Poluentes Ambientais , Ácidos Ftálicos , Humanos , Material Particulado/análise , Dietilexilftalato/análise , Ésteres/análise , Brasil , Ácidos Ftálicos/análise , Dibutilftalato/análise , Adipatos/análise , Poluentes Ambientais/análise
15.
Chemosphere ; 351: 141183, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38211793

RESUMO

Microplastics from mulch films can be a source of chemical contamination to agricultural soils. In this context, biodegradable films have been widely positioned as a greener choice. However, their sorption/desorption capabilities, in contrast to the conventional plastic types remain understudied. It is for this reason that objective evaluation of their interactions with residual agricultural contaminants becomes important. Our findings reveal that polyethylene (PE) mulch films retained lower amounts of pesticide residues and demonstrated a higher desorption/release [median desorption = 71.86 µg/L or about 50%], while polybutylene adipate terephthalate (PBAT) mulch films retained higher amounts of pesticide residues onto their surface and demonstrated a much lower desorption [median desorption = 24.27 µg/L or about 17%] after a spraying event. A higher ambient temperature had no significant effect on final desorption amounts in both PE [median = 65.27 µg/L at 20 °C and 74.23 µg/L at 40 °C] and PBAT [median = 24.26 µg/L at 20 °C and 24.78 µg/L at 40 °C] mulch films. However, it did favour a faster desorption pace in PE films. Desorption in PBAT and PE plastic types was correlated with the log Kow value [Spearman's correlation: 0.857 and 0.837 respectively, p < 0.05]. However, only a moderate correlation with pKa was observed in PBAT [Spearman's correlation: 0.478, p < 0.05], while none for PE plastic type. Sorption of pesticides onto biodegradable PBAT microplastics were best explained by Elovich [R2: 0.937-0.959] and pseudo-second order kinetics [R2: 0.942-0.987], suggesting the presence of chemisorption. Furthermore, Weber Morris plots suggested the presence of a multi-step process and Boyd plots indicated that film diffusion or chemical bond formation was the rate-limiting step governing this phenomenon.


Assuntos
Adipatos , Resíduos de Praguicidas , Praguicidas , Praguicidas/análise , Plásticos/química , Microplásticos , Agricultura , Solo/química , Polietileno
16.
Int J Biol Macromol ; 259(Pt 2): 129310, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38216014

RESUMO

Developing biobased materials is a considerably effective approach to save fossil resources and reduce emissions. Biobased polyamide 56 (PA56) is an excellent engineering material, but it has low toughness. Herein, to enhance the toughness of PA56, an ultra-tough biodegradable material, i.e., poly (butylene adipate-co-terephthalate) (PBAT) was introduced into PA56. Moreover, a self-synthesized epoxy-terminated hyperbranched polyester (EHBP) was used to improve the compatibility of the blended materials. The results of differential scanning calorimetry and Fourier-transform infrared spectroscopy indicated that the epoxide group of EHBP could react with PA56 and PBAT to form a block-like polymer structure and limit the crystallization behavior of the blends. The scanning electron microscopy results show that the addition of EHBP considerably reduced the dispersed-phase size in the blends, forming a nanoscale island structure. Moreover, the hydrogen bonds formed between EHBP and PA56/PBAT enhanced the intermolecular interaction between the two materials. Thus, PA56 blends with ultrahigh toughness were successfully prepared. The prepared PA56/PBAT/EHBP blend exhibited a notch impact strength of 20.71 kJ/m2 and a breaking elongation of 38.3 %, which represent increases of 427.3 % and 252.8 %, respectively, compared with those of pure PA56. Thus, the proposed method is suitable for toughening PA56 and broadening its applications.


Assuntos
Alcenos , Nylons , Ácidos Ftálicos , Polímeros , Poliésteres , Adipatos , Poli A
17.
Int J Biol Macromol ; 259(Pt 2): 129355, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38218295

RESUMO

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.


Assuntos
Alcenos , Peróxidos , Ácidos Ftálicos , Poliésteres , Polietilenoglicóis , Poliésteres/química , Adipatos/química
18.
Artigo em Inglês | MEDLINE | ID: mdl-38218565

RESUMO

Phthalate and non-phthalate plasticizers are used in polymer materials, such as plastic and rubber. It has recently been found that diisobutyl adipate (DIBA), which is considered an environmentally safe non-phthalate plasticizer, potentially acts as a thyroid disruptor in fish. Here, we investigated the sexual hormone effects of DIBA based on the expression levels of genes that respond to endocrine disruption and sexual hormone activity in the livers and gonads, and on gonadal sexual differentiation in Japanese medaka. Compared with the control group, the mRNA expression of chgH, vtg1, vtg2, and esr1 was significantly suppressed in the livers of DIBA exposed XX individuals. Furthermore, the mRNA expression of gsdf was significantly upregulated and downregulated in the gonads of XX and XY individuals, respectively. The mRNA expressions of esr1 and esr2b were significantly suppressed by DIBA exposure in the gonads of both XX and XY individuals. These observations suggest that DIBA has potential androgenic activity in Japanese medaka. However, normal testes and ovaries were observed in respective XY and XX medaka after DIBA exposure; therefore, these results suggest that DIBA may have weak androgenic activity.


Assuntos
Oryzias , Animais , Oryzias/genética , Oryzias/metabolismo , Diferenciação Sexual , Gônadas , Biomarcadores/metabolismo , Hormônios/metabolismo , RNA Mensageiro/genética , RNA Mensageiro/metabolismo , Adipatos/metabolismo , Adipatos/farmacologia
19.
Int J Biol Macromol ; 255: 127921, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37944741

RESUMO

To reduce the white pollution, the eco-friendly biodegradable poly (butylene adipate-co-terephthalate) (PBAT)-based films had attracted increasing interests worldwide. However, the high-cost of the PBAT had limited the large-scale development and application. In this work, 10 wt% low-cost lignin was introduced into the PBAT to prepare composite films by melt blending and blow molding, and the POSS(epoxy)8 was selected as the compatibilizer to improve the compatibility of PBAT and lignin. The maximum tensile strength and the nominal strain at break subsequently increased by 48.2 % and 21.4 % respectively, while the water vapor permeability enhanced by 9.9 %. Furthermore, the UV aging resistance of PBAT/lignin films were significantly improved, with only 1 wt% POSS(epoxy)8 content. This work provides an efficient strategy to foster the end-user confidence in the low-cost and eco-friendly biodegradable polymer materials with efficient performance.


Assuntos
Lignina , Poliésteres , Resinas Epóxi , Adipatos
20.
Mar Pollut Bull ; 199: 115947, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38157830

RESUMO

NPPs (Non-phthalate plasticizers) are used as alternative plasticizers to phthalate esters, but there is limited knowledge on environmental residues, and they have not been reported in Japan. A method to analyze NPPs in seawater using solid-phase extraction was developed, and the residual burden of Diisobutyl adipate (DIBA), Acetyl tributyl citrate (ATBC), Di-(2-ethylhexyl) adipate (DEHA), Di-(2-ethylhexyl) sebacate (DEHS) and Trioctyl trimellitate (TOTM) in seawater and sediment from the Osaka Bay was measured. Using an Oasis Max column and acetone as the eluting solvent, the recovery of the target substances in seawater is >68 %. In Osaka Bay, no NPPs were detected in seawater. On the other hand, ATBC and TOTM were detected in the sediment at 36-69 ng/g and 47-131 ng/g, respectively, from about half of the 14 sites, while DEHA and DEHS were detected at 83 ng/g and 181 ng/g, respectively, from only one site.


Assuntos
Benzoatos , Citratos , Ácidos Ftálicos , Plastificantes , Succinimidas , Plastificantes/análise , Ácidos Ftálicos/análise , Japão , Baías , Adipatos/análise , Água do Mar
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