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1.
J Transl Med ; 22(1): 51, 2024 01 13.
Artículo en Inglés | MEDLINE | ID: mdl-38216992

RESUMEN

BACKGROUND: Chest Computed tomography (CT) scans detect lung nodules and assess pulmonary fibrosis. While pulmonary fibrosis indicates increased lung cancer risk, current clinical practice characterizes nodule risk of malignancy based on nodule size and smoking history; little consideration is given to the fibrotic microenvironment. PURPOSE: To evaluate the effect of incorporating fibrotic microenvironment into classifying malignancy of lung nodules in chest CT images using deep learning techniques. MATERIALS AND METHODS: We developed a visualizable 3D classification model trained with in-house CT dataset for the nodule malignancy classification task. Three slightly-modified datasets were created: (1) nodule alone (microenvironment removed); (2) nodule with surrounding lung microenvironment; and (3) nodule in microenvironment with semantic fibrosis metadata. For each of the models, tenfold cross-validation was performed. Results were evaluated using quantitative measures, such as accuracy, sensitivity, specificity, and area-under-curve (AUC), as well as qualitative assessments, such as attention maps and class activation maps (CAM). RESULTS: The classification model trained with nodule alone achieved 75.61% accuracy, 50.00% sensitivity, 88.46% specificity, and 0.78 AUC; the model trained with nodule and microenvironment achieved 79.03% accuracy, 65.46% sensitivity, 85.86% specificity, and 0.84 AUC. The model trained with additional semantic fibrosis metadata achieved 80.84% accuracy, 74.67% sensitivity, 84.95% specificity, and 0.89 AUC. Our visual evaluation of attention maps and CAM suggested that both the nodules and the microenvironment contributed to the task. CONCLUSION: The nodule malignancy classification performance was found to be improving with microenvironment data. Further improvement was found when incorporating semantic fibrosis information.


Asunto(s)
Neoplasias Pulmonares , Fibrosis Pulmonar , Nódulo Pulmonar Solitario , Humanos , Neoplasias Pulmonares/patología , Fibrosis Pulmonar/complicaciones , Fibrosis Pulmonar/diagnóstico por imagen , Fibrosis Pulmonar/patología , Nódulo Pulmonar Solitario/diagnóstico por imagen , Nódulo Pulmonar Solitario/patología , Tomografía Computarizada por Rayos X/métodos , Pulmón/patología , Microambiente Tumoral
2.
J Transl Med ; 22(1): 67, 2024 01 16.
Artículo en Inglés | MEDLINE | ID: mdl-38229113

RESUMEN

PURPOSE: Evaluate the behavior of lung nodules occurring in areas of pulmonary fibrosis and compare them to pulmonary nodules occurring in the non-fibrotic lung parenchyma. METHODS: This retrospective review of chest CT scans and electronic medical records received expedited IRB approval and a waiver of informed consent. 4500 consecutive patients with a chest CT scan report containing the word fibrosis or a specific type of fibrosis were identified using the system M*Model Catalyst (Maplewood, Minnesota, U.S.). The largest nodule was measured in the longest dimension and re-evaluated, in the same way, on the follow-up exam if multiple time points were available. The nodule doubling time was calculated. If the patient developed cancer, the histologic diagnosis was documented. RESULTS: Six hundred and nine patients were found to have at least one pulmonary nodule on either the first or the second CT scan. 274 of the largest pulmonary nodules were in the fibrotic tissue and 335 were in the non-fibrotic lung parenchyma. Pathology proven cancer was more common in nodules occurring in areas of pulmonary fibrosis compared to nodules occurring in areas of non-fibrotic lung (34% vs 15%, p < 0.01). Adenocarcinoma was the most common cell type in both groups but more frequent in cancers occurring in non-fibrotic tissue. In the non-fibrotic lung, 1 of 126 (0.8%) of nodules measuring 1 to 6 mm were cancer. In contrast, 5 of 49 (10.2%) of nodules in fibrosis measuring 1 to 6 mm represented biopsy-proven cancer (p < 0.01). The doubling time for squamous cell cancer was shorter in the fibrotic lung compared to non-fibrotic lung, however, the difference was not statistically significant (p = 0.24). 15 incident lung nodules on second CT obtained ≤ 18 months after first CT scan was found in fibrotic lung and eight (53%) were diagnosed as cancer. CONCLUSIONS: Nodules occurring in fibrotic lung tissue are more likely to be cancer than nodules in the nonfibrotic lung. Incident pulmonary nodules in pulmonary fibrosis have a high likelihood of being cancer.


Asunto(s)
Neoplasias Pulmonares , Nódulos Pulmonares Múltiples , Fibrosis Pulmonar , Humanos , Neoplasias Pulmonares/diagnóstico por imagen , Neoplasias Pulmonares/patología , Fibrosis Pulmonar/diagnóstico por imagen , Fibrosis Pulmonar/patología , Nódulos Pulmonares Múltiples/patología , Pulmón/diagnóstico por imagen , Pulmón/patología , Tomografía Computarizada por Rayos X/métodos
3.
Environ Sci Technol ; 58(23): 10368-10377, 2024 Jun 11.
Artículo en Inglés | MEDLINE | ID: mdl-38814143

RESUMEN

The insect Tenebrio molitor exhibits ultrafast efficiency in biodegrading polystyrene (PS). However, the generation and fate of nanoplastics (NPs) in the intestine during plastic biodegradation remain unknown. In this study, we investigated the biodegradation of PS microplastics (MPs) mediated by T. molitor larvae over a 4-week period and confirmed biodegradation by analyzing Δδ13C in the PS before and after biotreatment (-28.37‰ versus -24.88‰) as an effective tool. The ·OH radicals, primarily contributed by gut microbiota, and H2O2, primarily produced by the host, both increased after MP digestion. The size distribution of residual MP particles in excrements fluctuated within the micrometer ranges. PS NPs were detected in the intestine but not in the excrements. At the end of Weeks 1, 2, 3, and 4, the concentrations of PS NPs in gut tissues were 3.778, 2.505, 2.087, and 2.853 ng/lava, respectively, while PS NPs in glands were quantified at 0.636, 0.284, and 0.113 ng/lava and eventually fell below the detection limit. The PS NPs in glands remained below the detection limit at the end of Weeks 5 and 6. This indicates that initially, NPs generated in the gut entered glands, then declined gradually and eventually disappeared or possibly biodegraded after Week 4, associated with the elevated plastic-degrading capacities of T. molitor larvae. Our findings unveil rapid synergistic MP biodegradation by the larval host and gut microbiota, as well as the fate of generated NPs, providing new insights into the risks and fate associated with NPs during invertebrate-mediated plastic biodegradation.


Asunto(s)
Biodegradación Ambiental , Larva , Microplásticos , Poliestirenos , Tenebrio , Animales , Microplásticos/metabolismo , Tenebrio/metabolismo , Larva/metabolismo , Plásticos/metabolismo , Microbioma Gastrointestinal
4.
Environ Sci Technol ; 2024 Jun 17.
Artículo en Inglés | MEDLINE | ID: mdl-38885123

RESUMEN

The detrimental effects of plastics on aquatic organisms, including those of macroplastics, microplastics, and nanoplastics, have been well established. However, knowledge on the interaction between plastics and terrestrial insects is limited. To develop effective strategies for mitigating the impact of plastic pollution on terrestrial ecosystems, it is necessary to understand the toxicity effects and influencing factors of plastic ingestion by insects. An overview of current knowledge regarding plastic ingestion by terrestrial insects is provided in this Review, and the factors influencing this interaction are identified. The pathways through which insects interact with plastics, which can lead to plastic accumulation and microplastic transfer to higher trophic levels, are also discussed using an overview and a conceptual model. The diverse impacts of plastic exposure on insects are discussed, and the challenges in existing studies, such as a limited focus on certain plastic types, are identified. Further research on standardized methods for sampling and analysis is crucial for reliable research, and long-term monitoring is essential to assess plastic trends and ecological impacts in terrestrial ecosystems. The mechanisms underlying these effects need to be uncovered, and their potential long-term consequences for insect populations and ecosystems require evaluation.

5.
Angew Chem Int Ed Engl ; 63(7): e202314685, 2024 Feb 12.
Artículo en Inglés | MEDLINE | ID: mdl-38158892

RESUMEN

Semicrystalline polymer dielectrics (SPDs) are highly sought-after state-of-the-art dielectric materials. As the disorder in SPDs degrades their electrical properties, homogeneously ordered SPDs are desired. However, complex crystallization behaviors of polymers make such homogeneity elusive. Polymer lamellar single crystals (PLSCs), the most regularly-ordered form of SPDs possible under mild crystallizing conditions, are ideal platforms for understanding and developing high-performance dielectric materials. Here, a typical and widely used SPD, polyethylene (PE) is selected as the model material. We successfully obtained, large, uniform, and high-quality PE PLSCs and devised a non-destructive strategy to construct PE PLSC-based vertical capacitors. These nanometer-thick capacitors exhibit exceptional dielectric properties, with a high breakdown strength of 6.95 MV/cm and a low dielectric constant of 2.14±0.07, that outperform the properties of any existing neat PE. This work provides novel insights into exploring the performance possibility of ordered SPDs and reveals the PLSCs as potential high-performance dielectric materials.

6.
Environ Sci Technol ; 57(40): 15099-15111, 2023 10 10.
Artículo en Inglés | MEDLINE | ID: mdl-37751481

RESUMEN

It remains unknown whether plastic-biodegrading macroinvertebrates generate microplastics (MPs) and nanoplastics (NPs) during the biodegradation of plastics. In this study, we utilized highly sensitive particle analyzers and pyrolyzer-gas chromatography mass spectrometry (Py-GCMS) to investigate the possibility of generating MPs and NPs in frass during the biodegradation of polystyrene (PS) and low-density polyethylene (LDPE) foams by mealworms (Tenebrio molitor larvae). We also developed a digestive biofragmentation model to predict and unveil the fragmentation process of ingested plastics. The mealworms removed 77.3% of ingested PS and 71.1% of ingested PE over a 6-week test period. Biodegradation of both polymers was verified by the increase in the δ13C signature of residual plastics, changes in molecular weights, and the formation of new oxidative functional groups. MPs accumulated in the frass due to biofragmentation, with residual PS and PE exhibiting the maximum percentage by number at 2.75 and 7.27 µm, respectively. Nevertheless, NPs were not detected using a laser light scattering sizer with a detection limit of 10 nm and Py-GCMS analysis. The digestive biofragmentation model predicted that the ingested PS and PE were progressively size-reduced and rapidly biodegraded, indicating the shorter half-life the smaller plastic particles have. This study allayed concerns regarding the accumulation of NPs by plastic-degrading mealworms and provided critical insights into the factors controlling MP and NP generation during macroinvertebrate-mediated plastic biodegradation.


Asunto(s)
Poliestirenos , Tenebrio , Animales , Polietileno , Tenebrio/metabolismo , Plásticos , Larva/metabolismo , Biodegradación Ambiental , Microplásticos
7.
J Environ Manage ; 345: 118818, 2023 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-37633102

RESUMEN

It is widely understood that microplastics (MPs) can induce various biological stresses in macroinvertebrates that are incapable of biodegrading plastics. However, the biodegradation and physiological responses of plastic-degrading macroinvertebrates toward MPs of different degradability levels remain unexplored. In this study, Tenebrio molitor larvae (mealworms) were selected as a model of plastics-degrading macroinvertebrate, and were tested against three common plastics of different degradability rankings: polyvinyl chloride (PVC), polystyrene (PS), and polylactic acid (PLA) MPs (size <300 µm). These three MPs were biodegraded with the rate sequence of PLA > PS > PVC, resulting in a reversed order of negative physiological responses (body weight loss, decreased survival, and biomass depletion) of mealworms. Simultaneously, the levels of reactive oxygen species (ROS), antioxidant enzyme activities, and lipid peroxidation were uniformly increased as polymer degradability decreased and intermediate toxicity increased. PVC MPs exhibited higher toxicity than the other two polymers. The oxidative stresses were effectively alleviated by supplementing co-diet bran. The T. molitor larvae fed with PLA plus bran showed sustainable growth without an increase in oxidative stress. The results provide new insights into the biotoxicity of MPs on macroinvertebrates and offer comprehensive information on the physiological stress responses of plastic-degrading macroinvertebrates during the biodegradation of plastics with different degradability levels.


Asunto(s)
Poliestirenos , Tenebrio , Animales , Poliestirenos/toxicidad , Larva/metabolismo , Tenebrio/metabolismo , Plásticos , Microplásticos/toxicidad , Microplásticos/metabolismo , Cloruro de Polivinilo , Poliésteres/metabolismo , Antioxidantes/metabolismo
8.
Small ; 18(8): e2106066, 2022 02.
Artículo en Inglés | MEDLINE | ID: mdl-34881811

RESUMEN

In the development of flexible organic field-effect transistors (OFET), downsizing and reduction of the operating voltage are essential for achieving a high current density with a low operating power. Although the bias voltage of the OFETs can be reduced by a high-k dielectric, achieving a threshold voltage close to zero remains a challenge. Moreover, the scaling down of OFETs demands the use of photolithography, and may lead to compatibility issues in organic semiconductors. Herein, a new strategy based on the ductile properties of organic semiconductors is developed to control the threshold voltage at close to zero while concurrently downsizing the OFETs. The OFETs are fabricated on prestressed polystyrene shrink film substrates at room temperature, then thermal energy (160 °C) is used to release the strain. The OFETs conformally attached to the wrinkled structure are shown to locally amplify the electric field. After shrinking, the horizontal device area is reduced by 75%, and the threshold voltage is decreased from -1.44 to -0.18 V, with a subthreshold swing of 74 mV dec-1 and intrinsic gain of 4.151 × 104 . These results reveal that the shrink film can be generally used as a substrate for downsizing OFETs and improving their performance.


Asunto(s)
Semiconductores , Transistores Electrónicos
9.
Acc Chem Res ; 54(24): 4498-4507, 2021 Dec 21.
Artículo en Inglés | MEDLINE | ID: mdl-34866378

RESUMEN

ConspectusSingle crystals of organic semiconductors (OSCs) are believed to have both high mobility and intrinsic flexibility, making them promising candidates for flexible electronic/optoelectronic applications and being consistently pursued by researchers. The van der Waals force in OSC enables low-temperature solution processing of single crystals, but the relatively weak binding energy brings challenges in forming large, uniform, and defect-free single crystals. To promote the study on OSC single crystals, a generalized method that grows high-quality crystals in an easy-to-handle, time/resource-saving, and repeatable manner is apparently necessary. In 2012, Li et al. developed a droplet-pinned crystallization (DPC) method that uses a rather simple strategy to create a steadily receding contact line for the growth of OSC single crystals. Instead of setting up expensive equipment, controlling strict deposition parameters, or waiting for days or weeks for countable crystal seeds, the DPC method offers a time- and cost-effective way to obtain OSC single crystals for further study of the tendency of crystallization, single-crystal mobility, and molecular packing information. The DPC method is primarily a powerful tool for studying the charge-transport mechanisms in OSC single crystals. In pioneering work, high-mobility single crystals of both p-type 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS-PEN) and n-type C60 materials were obtained. Driven by the demands from practical applications, we then focused on the general lagging of electron mobility in OSC materials. The ambipolar property of TIPS-PEN was studied, and a strong correlation between electron mobility and polar species (polar solvent residuals and surface hydroxyl groups) was observed. The latter further guided the harvest of electron mobility in a series of OSC materials. Undoubtfully, the facile DPC method accelerated these studies by providing a time-efficient, reliable, and repeatable testing platform. Additionally, flexibility on OSC materials and solvents, where not only one-component but also binary systems were allowed, is another critical integrity of the DPC method. The m-xylene/carbon tetrachloride binary solvent was proven to be efficient for growing ribbon-like C60 single crystals rather than needle-like crystals from typical one-component solvents. Afterward, a variety of OSC materials (including p-type, n-type, and ambipolar ones) and a series of solvents (including aromatic, aliphatic, and polar ones) were studied. The crystallization of OSC single crystals was primarily found at either the top liquid-air interface or the bottom solid-liquid interface. The interactions between OSC molecules and substrate surfaces were deduced as the qualitative determining factor. By utilizing the top interface crystallization, the two-step sequential deposition of single-crystalline OSC heterojunctions was enabled. Moreover, by selecting appropriate pairs of OSC materials that crystallize at separate interfaces, the facile one-step formation of single-crystalline OSC heterojunctions was achieved. The OSC single crystals and heterojunctions (including horizontal, vertical, and bulk heterojunctions) thereof exhibit promising potentials in circuits, photovoltaics, and photodiodes and would probably provide new insights for the future development of organic electronics.

10.
NMR Biomed ; 35(8): e4739, 2022 08.
Artículo en Inglés | MEDLINE | ID: mdl-35393706

RESUMEN

B0 inhomogeneity leads to imaging artifacts in cardiac magnetic resonance imaging (MRI), in particular dark band artifacts with steady-state free precession pulse sequences. The limited spatial resolution of MR-derived in vivo B0 maps and the lack of population data prevent systematic analysis of the problem at hand and the development of optimized B0 shim strategies. We used readily available clinical computed tomography (CT) images to simulate the B0 conditions in the human heart at high spatial resolution. Calculated B0 fields showed consistency with MRI-based B0 measurements. The B0 maps for both the simulations and in vivo measurements showed local field inhomogeneities in the vicinity of lung tips with dominant Z3 spherical harmonic terms in the field distribution. The presented simulation approach allows for the derivation of B0 field conditions at high spatial resolution from CT images and enables the development of subject- and population-specific B0 shim strategies for the human heart.


Asunto(s)
Encéfalo , Imagen por Resonancia Magnética , Artefactos , Corazón/diagnóstico por imagen , Humanos , Procesamiento de Imagen Asistido por Computador/métodos , Imagen por Resonancia Magnética/métodos , Tomografía Computarizada por Rayos X
11.
Environ Sci Technol ; 56(23): 17310-17320, 2022 12 06.
Artículo en Inglés | MEDLINE | ID: mdl-36350780

RESUMEN

Biodegradation of polystyrene (PS) in mealworms (Tenebrio molitor lavae) has been identified with commercial PS foams. However, there is currently limited understanding of the influence of molecular weight (MW) on insect-mediated plastic biodegradation and the corresponding responses of mealworms. In this study, we provided the results of PS biodegradation, gut microbiome, and metabolome by feeding mealworms with high-purity PS microplastics with a wide variety of MW. Over 24 days, mealworms (50 individuals) fed with 0.20 g of PS showed decreasing removal of 74.1 ± 1.7, 64.1 ± 1.6, 64.4 ± 4.0, 73.5 ± 0.9, 60.6 ± 2.6, and 39.7 ± 4.3% for PS polymers with respective weight-average molecular weights (Mw) of 6.70, 29.17, 88.63, 192.9, 612.2, and 1346 kDa. The mealworms degraded most PS polymers via broad depolymerization but ultrahigh-MW PS via limited-extent depolymerization. The gut microbiome was strongly associated with biodegradation, but that with low- and medium-MW PS was significantly distinct from that with ultrahigh-MW PS. Metabolomic analysis indicated that PS biodegradation reprogrammed the metabolome and caused intestinal dysbiosis depending on MW. Our findings demonstrate that mealworms alter their gut microbiome and intestinal metabolic pathways in response to in vivo biodegradation of PS polymers of various MWs.


Asunto(s)
Microbioma Gastrointestinal , Tenebrio , Humanos , Animales , Tenebrio/metabolismo , Poliestirenos , Plásticos , Microbioma Gastrointestinal/fisiología , Peso Molecular , Polímeros , Larva/metabolismo , Metaboloma
12.
J Comput Assist Tomogr ; 46(3): 423-433, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-35405687

RESUMEN

OBJECTIVE: This study aimed to calculate scanner-, kilovoltage peak (kVp)-, and patient size-specific computed tomography (CT) number thresholds for determining Agatston score (AgSc). METHODS: The proposed method was validated using calcium measurements in an anthropomorphic phantom for 4 CT scanners made by 4 vendors. The derived mass concentration (γ) thresholds were used to calculate kVp- and patient size-specific CT number thresholds. Two models were applied to reduce intrascanner and interscanner AgSc variation, respectively. RESULTS: The mean error of the modeled CT numbers is 1.8% (0.1%-4.4%). Model 1 has comparable results to the published phantom calibration method for an average-size patient (error, 1.5%; 0.1%-5.1%). The size- and the kVp-dependent fitting of modeled results have R2 greater than 0.965. CONCLUSIONS: Our results show a potential to enable accurate determination of AgSc under diverse conditions (eg, reduced tube potential) and are more easily applicable to different patient sizes than the phantom calibration method.


Asunto(s)
Tomografía Computarizada por Rayos X , Calibración , Humanos , Fantasmas de Imagen , Reproducibilidad de los Resultados , Tomógrafos Computarizados por Rayos X , Tomografía Computarizada por Rayos X/métodos
13.
Environ Sci Technol ; 53(9): 5256-5265, 2019 05 07.
Artículo en Inglés | MEDLINE | ID: mdl-30990998

RESUMEN

Yellow mealworms (larvae of Tenebrio molitor, Coleoptera: Tenebrionidae) have been proven to be capable of biodegrading polystyrene (PS) products. Using four geographic sources, we found that dark mealworms (larvae of Tenebrio obscurus) ate PS as well. We subsequently tested T. obscurus from Shandong, China for PS degradation capability. Our results demonstrated the ability for PS degradation within the gut of T. obscurus at greater rates than T. molitor. With expanded PS foam as the sole diet, the specific PS consumption rates for T. obscurus and T. molitor at similar sizes (2.0 cm, 62-64 mg per larva) were 32.44 ± 0.51 and 24.30 ± 1.34 mg 100 larvae-1 d-1, respectively. After 31 days, the molecular weight ( Mn) of residual PS in frass (excrement) of T. obscurus decreased by 26.03%, remarkably higher than that of T. molitor (11.67%). Fourier transform infrared spectroscopy (FTIR) indicated formation of functional groups of intermediates and chemical modification. Thermo gravimetric analysis (TGA) suggested that T. obscurus larvae degraded PS effectively based on the proportion of PS residue. Co-fed corn flour to T. obscurus and wheat bran to T. molitor increased total PS consumption by 11.6% and 15.2%, respectively. Antibiotic gentamicin almost completely inhibited PS depolymerization. High-throughput sequencing revealed significant shifts in the gut microbial community in both Tenebrio species that were associated with the PS diet and PS biodegradation, with changes in three predominant families (Enterobacteriaceae, Spiroplasmataceae, and Enterococcaceae). The results indicate that PS biodegradability may be ubiquitous within the Tenebrio genus which could provide a bioresource for plastic waste biodegradation.


Asunto(s)
Escarabajos , Tenebrio , Animales , Biodegradación Ambiental , China , Larva , Poliestirenos
14.
Water Res ; 259: 121841, 2024 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-38820734

RESUMEN

The toxicity of microplastics (MPs) on freshwater plants has been widely studied, yet the influence of aged MPs remains largely unexplored. Herein, we investigated the influence of polyvinyl chloride (PVC) MPs, both before and after aging, at different environmentally relevant concentrations on Chlorella pyrenoidosa, a freshwater microalgae species widely recognized as a valuable biomass resource. During a 96-h period, both virgin and aged MPs hindered the growth of C. pyrenoidosa. The maximum growth inhibition rates were 32.40 % for virgin PVC at 250 mg/L and 44.72 % for aged PVC at 100 mg/L, respectively. Microalgae intracellular materials, i.e., protein and carbohydrate contents, consistently decreased after MP exposure, with more pronounced inhibition observed with aged PVC. Meanwhile, the MP aging significantly promoted the nitrogen uptake of C. pyrenoidosa, i.e., 1693.45 ± 42.29 mg/L (p < 0.01), contributing to the production of humic acid-like substances. Additionally, aged PVC induced lower chlorophyll a and Fv/Fm when compared to virgin PVC, suggesting a more serious inhibition of the photosynthesis process of microalgae. The toxicity of MPs to C. pyrenoidosa was strongly associated with intercellular oxidative stress levels. The results indicate that MP aging exacerbates the damage to photosynthetic performance and bioenergy production in microalgae, providing critical insights into the toxicity analysis of micro(nano)plastics on freshwater plants.


Asunto(s)
Chlorella , Microalgas , Microplásticos , Fotosíntesis , Fotosíntesis/efectos de los fármacos , Chlorella/efectos de los fármacos , Microalgas/efectos de los fármacos , Microplásticos/toxicidad , Contaminantes Químicos del Agua/toxicidad , Biomasa , Clorofila/metabolismo
15.
J Hazard Mater ; 465: 133446, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38219578

RESUMEN

Polyethylene terephthalate (PET or polyester) is a commonly used plastic and also contributes to the majority of plastic wastes. Mealworms (Tenebrio molitor larvae) are capable of biodegrading major plastic polymers but their degrading ability for PET has not been characterized based on polymer chain size molecular size, gut microbiome, metabolome and transcriptome. We verified biodegradation of commercial PET by T. molitor larvae in a previous report. Here, we reported that biodegradation of commercial PET (Mw 29.43 kDa) was further confirmed by using the δ13C signature as an indication of bioreaction, which was increased from - 27.50‰ to - 26.05‰. Under antibiotic suppression of gut microbes, the PET was still depolymerized, indicating that the host digestive enzymes could degrade PET independently. Biodegradation of high purity PET with low, medium, and high molecular weights (MW), i.e., Mw values of 1.10, 27.10, and 63.50 kDa with crystallinity 53.66%, 33.43%, and 4.25%, respectively, showed a mass reduction of > 95%, 86%, and 74% via broad depolymerization. Microbiome analyses indicated that PET diets shifted gut microbiota to three distinct structures, depending on the low, medium, and high MW. Metagenome sequencing, transcriptomic, and metabolic analyses indicated symbiotic biodegradation of PET by the host and gut microbiota. After PET was fed, the host's genes encoding degradation enzymes were upregulated, including genes encoding oxidizing, hydrolyzing, and non-specific CYP450 enzymes. Gut bacterial genes for biodegrading intermediates and nitrogen fixation also upregulated. The multiple-functional metabolic pathways for PET biodegradation ensured rapid biodegradation resulting in a half-life of PET less than 4 h with less negative impact by PET MW and crystallinity.


Asunto(s)
Tenebrio , Animales , Tenebrio/metabolismo , Tenebrio/microbiología , Poliestirenos/metabolismo , Tereftalatos Polietilenos/metabolismo , Polímeros , Larva/metabolismo , Polietileno/metabolismo , Plásticos/metabolismo , Biodegradación Ambiental , Metaboloma
16.
Org Lett ; 25(15): 2606-2610, 2023 Apr 21.
Artículo en Inglés | MEDLINE | ID: mdl-37039345

RESUMEN

The mild and efficient palladium-catalyzed pyrrolidin-2-yl and tetrahydrofuran-2-yl methylation of (hetero)arenes has been developed. A wide range of (hetero)arenes underwent the regioselective thianthrenation to generate the arylthianthrenium triflate, and the developed Pd-catalyzed alkene carboamination and carboalkoxylation reactions afforded the corresponding biologically important pyrrolidine and tetrahydrofuran derivatives. Mechanistic studies indicated that this reaction proceeds through a syn-heteropalladation mechanistic pathway. The demonstrated late-stage functionalization and enantioselective reaction will help to promote the potential application of the established method in organic synthesis and related fields.

17.
Adv Mater ; 35(52): e2304736, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37494287

RESUMEN

Despite remarkable improvement in the mobility of the organic field-effect transistors (OFETs) being achieved in past decades, the uniformity in electrical performance remains ambiguous, impeding their implantation in organic integrated circuits. The coefficient of variance (CV) in mobility of reported OFETs is typically larger than 8%, which is not adequate for building medium-to-large scale integrated circuits. In this work, it is shown that utilizing single-domain molecular monolayer crystals as the active channel can largely enhance the uniformity of OFETs. Benefiting from the sole molecular layer with long-range ordering, the OFETs exhibit uniformities in both channel transport and charge injection, thereby giving rise to a high average mobility of 11.64 cm2 V-1 s-1 and CV of only 2.57%. Statistical transmission length method evaluation is conducted, covering channel length from 3 to 21 µm, channel width from 90 to 170 µm, and a total OFET number of 370. The low contact resistance of 79.00 ± 7.00 Ω cm and high intrinsic mobility of 12.36 ± 0.45 cm2 V-1 s-1 are acquired with very high accuracy and reliability. As such, this work provides a practical way to enhance the uniformity of OFETs by a single-crystalline layer-controlled active channel toward their applications in integrated circuits.

18.
Nanoscale ; 15(47): 19099-19109, 2023 Dec 07.
Artículo en Inglés | MEDLINE | ID: mdl-37961946

RESUMEN

Understanding the correlation mechanism of side chains on thermal transport of organic semiconductors is crucial for functionalized organic electronics. In this study, phenyl and alkyl side chains, two representatives of side chain engineering, are chosen to modify dinaphtho-[2,3-b:2',3'-f]thieno[3,2-b]thiophene (DNTT) to synthesize Ph-DNTT and C10-DNTT. The thermal conductivities of the three organic semiconductors exhibit obvious anisotropy, and the corresponding relationships are along-chain > inter-chain > cross-chain. The phenyl side chains enhance the thermal conductivity in the along-chain direction and degrade it in the inter-chain direction, while the alkyl side chains hinder thermal transport. In the cross-chain direction, side chains have a slight effect on thermal transport. The structure orientation consistency between the phenyl side chains and the main chains in Ph-DNTT leads to phonon coupling in the along-chain direction, which improves phonon transport. In the inter-chain direction, the combined effect of the phonon group velocity and phonon participation ratio causes the thermal conductivity degeneracy of Ph-DNTT. For C10-DNTT, the vibrational mismatch between the alkyl side chains and the main chains results in the degradation of thermal transport in the along-chain and inter-chain directions. In the cross-chain direction, the nonbonding interaction dominates the energy transfer in the three organic semiconductors, which induces inferior phonon transport properties and weak effects of side chains.

19.
Sci Total Environ ; 863: 160866, 2023 Mar 10.
Artículo en Inglés | MEDLINE | ID: mdl-36526173

RESUMEN

As the application of biodegradable polymers has grown, so has the interest in exploring the environmental behaviors of biodegradable microplastics (MPs). In this study, we investigated the interaction of oxytetracycline (OTC) with poly(butylene adipate-co-terephthalate) (PBAT) MPs after biodegradation, and explored the effect of the coexisting Cu(II) on OTC adsorption and desorption processes. The maximum adsorption amounts of virgin PBAT, biofilm PBAT, and degraded PBAT reached 692.05 µg·g-1, 1396.21 µg·g-1, and 1869.93 µg·g-1, respectively, and the presence of Cu(II) increased the OTC adsorption capacities by 431.16 %, 165.99 %, and 132.94 %, respectively. The enhanced adsorption capacities were attributed to the formation of PBAT-Cu-OTC complexes. The remarkable desorption hysteresis of OTC was observed on the degraded PBAT but not on the biofilm PBAT when Cu(II) was present, due to the complexation between Cu(II) and biofilms. The effect of Cu(II) varied depending on the MP physiochemical properties (e.g., surface areas, zeta potentials, and functional groups) and the environmental factors (e.g., the solution pH and coexisting dissolved organic matter). Fourier transform infrared spectroscopy (FTIR) coupled with X-ray photoelectron spectroscopy (XPS) identified the Cu(II) bridging effect, and various interaction forces between PBAT and OTC, including hydrogen-bonding, π-π, cation-π, and electrostatic interactions.


Asunto(s)
Microplásticos , Oxitetraciclina , Plásticos , Poliésteres/química , Materia Orgánica Disuelta , Agua , Adsorción , Adipatos , Concentración de Iones de Hidrógeno
20.
Sci Total Environ ; 859(Pt 2): 160237, 2023 Feb 10.
Artículo en Inglés | MEDLINE | ID: mdl-36402329

RESUMEN

Wastewater recycling helps address the challenge of microalgae biomass commercialization by allowing for efficient resource recovery. In this study, three conventional harvesting methods, including centrifugation, microfiltration, and flocculation sedimentation, were investigated to explore the effects of harvesting methods on the characteristics of recycled wastewater and the growth of microalgae to select a suitable harvesting method for the microalgal wastewater recycling system. During the wastewater recycling process, the least amount of accumulated substances was exhibited in the wastewater recycled by microfiltration, followed by centrifugation, and the most by flocculation sedimentation. After 4 batches of cultivation, microalgal biomass harvested from centrifugation wastewater and microfiltration wastewater was 21.26 % and 13.54 % higher than that from flocculation wastewater, respectively. Lipids, carbohydrates and pigments were all increased by varying degrees. Additionally, flocculation sedimentation was not suitable for the microalgal wastewater recycling process since the low residual nutrients, high salinity, and excessive algal organic matter severely inhibited the growth of microalgae. Under the regulation of phytohormones, microalgae increased their energy reserves, enhanced photosynthesis, and improved their defense capability to resist the increasing abiotic stress. This study provides scientific support for the selection of suitable harvesting technology during the microalgal wastewater recycling process.


Asunto(s)
Microalgas , Aguas Residuales , Floculación , Biomasa , Reciclaje
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