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1.
J Nat Prod ; 87(4): 837-848, 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38417401

RESUMO

Ovarian cancer (OVC) is one of the most aggressive gynecological malignancies worldwide. Although olaparib treatment has shown favorable outcomes against the treatment of OVC, its effectiveness remains limited in some OVC patients. Investigating new strategies to improve the therapeutic efficacy of olaparib against OVC is imperative. Our study identified tabersonine, a natural indole alkaloid, for its potential to increase the chemosensitivity of olaparib in OVC. The combined treatment of olaparib and tabersonine synergistically inhibited cell proliferation in OVC cells and suppressed tumor growth in A2780 xenografts. The combined treatment effectively suppressed epithelial-mesenchymal transition (EMT) by altering the expression of E-cadherin, N-cadherin, and vimentin and induced DNA damage responses. Integrating quantitative proteomics, FHL1 was identified as a potential regulator to modulate EMT after tabersonine treatment. Increased expression of FHL1 was induced by tabersonine treatment, while downregulation of FHL1 reversed the inhibitory effects of tabersonine on OVC cells by mediating EMT. In vivo findings further reflected that the combined treatment of tabersonine and olaparib significantly inhibited tumor growth and OVC metastasis through upregulation of FHL1. Our findings reveal the role of tabersonine in improving the sensitivity of olaparib in OVC through FHL1-mediated EMT, suggesting that tabersonine holds promise for future application in OVC treatment.


Assuntos
Transição Epitelial-Mesenquimal , Peptídeos e Proteínas de Sinalização Intracelular , Proteínas com Domínio LIM , Proteínas Musculares , Neoplasias Ovarianas , Ftalazinas , Piperazinas , Animais , Feminino , Humanos , Camundongos , Antineoplásicos/farmacologia , Linhagem Celular Tumoral , Proliferação de Células/efeitos dos fármacos , Transição Epitelial-Mesenquimal/efeitos dos fármacos , Alcaloides Indólicos/farmacologia , Peptídeos e Proteínas de Sinalização Intracelular/metabolismo , Proteínas Musculares/metabolismo , Proteínas Musculares/efeitos dos fármacos , Neoplasias Ovarianas/tratamento farmacológico , Neoplasias Ovarianas/patologia , Ftalazinas/farmacologia , Piperazinas/farmacologia , Quinolinas/farmacologia
2.
Environ Res ; 243: 117813, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-38043893

RESUMO

Terrestrial gross primary production (GPP) changes due to impervious surfaces significantly impact ecosystem services in watersheds. Understanding the asymmetric response of vegetation GPP to impervious surface expansion is essential for regional development planning and ecosystem management. However, the asymmetric response of vegetation GPP to the impacts of impervious surface expansion is unknown in different watersheds. This paper selected the Yellow River and Yangtze River basins as case studies. We characterized the overall change in GPP based on changes in impervious surface ratio (ISR), determined impervious surface expansion's direct and indirect impacts on GPP in the two watersheds, and further analyzed the asymmetric response of the compensatory effects of indirect influences on the impervious surface expansion in different watersheds. The results showed that: (1) The vegetation GPP decreased with increasing ISR in the Yangtze River Basin, while that in the Yellow River Basin first increased and then reduced. (2) The direct impacts of increased ISR reduced vegetation GPP, while the indirect impacts both had a growth-compensating effect. Growth compensation stabilized at approximately 0.40 and 0.30 in the Yellow and Yangtze River Basins. (3) When the ISR was 0.34-0.56, the growth compensation could offset the reduction of GPP due to direct impact and ensure that the background vegetation GPP was not damaged in the Yellow River Basin. In contrast, the background vegetation GPP was inevitably impaired with increased ISR in the Yangtze River Basin. Therefore, this study suggests that the ISR should be ensured to be between 0.34 and 0.56 to maximize the impervious surface of the Yellow River Basin without compromising the background vegetation GPP. While pursuing impervious surface expansion in the Yangtze River Basin, other programs should be sought to compensate for the loss to GPP.


Assuntos
Ecossistema , Monitoramento Ambiental , Rios , China
3.
Sensors (Basel) ; 24(10)2024 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-38794077

RESUMO

Sensors are a key component in industrial automation systems. A fault or malfunction in sensors may degrade control system performance. An engineering system model is usually disturbed by input uncertainties, which brings a challenge for monitoring, diagnosis, and control. In this study, a novel estimation technique, called adaptive unknown-input observer, is proposed to simultaneously reconstruct sensor faults as well as system states. Specifically, the unknown input observer is used to decouple partial disturbances, the un-decoupled disturbances are attenuated by the optimization using linear matrix inequalities, and the adaptive technique is explored to track sensor faults. As a result, a robust reconstruction of the sensor fault as well as system states is then achieved. Furthermore, the proposed robustly adaptive fault reconstruction technique is extended to Lipschitz nonlinear systems subjected to sensor faults and unknown input uncertainties. Finally, the effectiveness of the algorithms is demonstrated using an aircraft system model and robotic arm and comparison studies.

4.
Pharm Biol ; 62(1): 394-403, 2024 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38739003

RESUMO

CONTEXT: Tabersonine has been investigated for its role in modulating inflammation-associated pathways in various diseases. However, its regulatory effects on triple-negative breast cancer (TNBC) have not yet been fully elucidated. OBJECTIVE: This study uncovers the anticancer properties of tabersonine in TNBC cells, elucidating its role in enhancing chemosensitivity to cisplatin (CDDP). MATERIALS AND METHODS: After tabersonine (10 µM) and/or CDDP (10 µM) treatment for 48 h in BT549 and MDA-MB-231 cells, cell proliferation was evaluated using the cell counting kit-8 and colony formation assays. Quantitative proteomics, online prediction tools and molecular docking analyses were used to identify potential downstream targets of tabersonine. Transwell and wound-healing assays and Western blot analysis were used to assess epithelial-mesenchymal transition (EMT) phenotypes. RESULTS: Tabersonine demonstrated inhibitory effects on TNBC cells, with IC50 values at 48 h being 18.1 µM for BT549 and 27.0 µM for MDA-MB-231. The combined treatment of CDDP and tabersonine synergistically suppressed cell proliferation in BT549 and MDA-MB-231 cells. Enrichment analysis revealed that the proteins differentially regulated by tabersonine were involved in EMT-related signalling pathways. This combination treatment also effectively restricted EMT-related phenotypes. Through the integration of online target prediction and proteomic analysis, Aurora kinase A (AURKA) was identified as a potential downstream target of tabersonine. AURKA expression was reduced in TNBC cells post-treatment with tabersonine. DISCUSSION AND CONCLUSIONS: Tabersonine significantly enhances the chemosensitivity of CDDP in TNBC cells, underscoring its potential as a promising therapeutic agent for TNBC treatment.


Assuntos
Aurora Quinase A , Cisplatino , Transição Epitelial-Mesenquimal , Alcaloides Indólicos , Neoplasias de Mama Triplo Negativas , Feminino , Humanos , Antineoplásicos/farmacologia , Aurora Quinase A/metabolismo , Linhagem Celular Tumoral , Proliferação de Células/efeitos dos fármacos , Cisplatino/farmacologia , Sinergismo Farmacológico , Transição Epitelial-Mesenquimal/efeitos dos fármacos , Alcaloides Indólicos/farmacologia , Simulação de Acoplamento Molecular , Neoplasias de Mama Triplo Negativas/tratamento farmacológico , Neoplasias de Mama Triplo Negativas/patologia
5.
Biochem Biophys Res Commun ; 673: 160-168, 2023 09 17.
Artigo em Inglês | MEDLINE | ID: mdl-37392479

RESUMO

Atopic dermatitis (AD) is a common disease with a considerable impact on the patient's quality of life and limited treatment options. Sodium thiosulfate (STS) is a traditional medicine used in the rescue of cyanide poisoning, and some pruritus dermatosis. However, the exact efficacy and mechanism of its application on AD are not clear. In this work, comparing to other traditional therapy, STS was found to effectively improve the severity of skin lesions and the quality of life in AD patients with a dose-dependent manner. Mechanically, STS downregulated the expression of IL-4, IL-13, IgE in the serum of AD patients, as well as reduce the concentration of eosinophils. Furthermore, in the AD-like mice model triggered by ovalbumin (OVA) and calcitriol, STS was found to reduce the epidermal thickness, scratching times, and the infiltration of dermal inflammatory cells in AD mice, as well as the reactive oxygen species (ROS) production and the expression levels of inflammatory cytokines in the skin tissue. In HacaT cells, STS inhibited the accumulation of ROS and activation of NLRP3 inflammasome and its downstream IL-1ß expression. Therefore, this study revealed that STS plays an important therapeutic role in AD, and the mechanism may be that STS inhibits the activation of NLRP3 inflammasome and the subsequent release of inflammatory cytokines. Thus, the role of STS in treating AD was clarified and the possible molecular mechanism was revealed.


Assuntos
Dermatite Atópica , Animais , Camundongos , Citocinas/metabolismo , Dermatite Atópica/patologia , Modelos Animais de Doenças , Inflamassomos , Camundongos Endogâmicos BALB C , Proteína 3 que Contém Domínio de Pirina da Família NLR/metabolismo , Qualidade de Vida , Espécies Reativas de Oxigênio , Pele/patologia
6.
Int Arch Allergy Immunol ; 184(1): 43-53, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36279853

RESUMO

INTRODUCTION: The effect of the COVID-19 pandemic on allergic diseases is not certain, as people's living habits and the environment have been affected by the pandemic. The present study described the influence of the COVID-19 pandemic on the allergen sensitization rate in patients with allergic diseases in central China. The results provide reliable epidemiological data for the prevention and control of allergic diseases during the COVID-19 epidemic. METHODS: Data were collected from a total of 6,915 patients with symptoms of allergic diseases who visited the Third Xiangya Hospital of Central South University in China for allergen testing from January 1, 2018, to December 31, 2021. Patients were divided into a children group (<14 years old), youth group (15∼44 years old), middle-aged group (45∼59 years old), and elderly group (>60 years old). Immunoblotting was used to detect 20 serum allergen-specific IgE (sIgE) antibodies in patient serum samples. We compared the positive rates of various allergens in different age and sex groups before and during the COVID-19 epidemic, and the prevalence data of sIgE sensitization were analysed. RESULTS: Among the 6,915 patients with symptoms of allergic diseases, 2,838 (41.04%) patients were positive for at least one of the allergens. The top three positive rates of inhaled allergens were Dermatophagoides farinae (1,764 cases, 25.51%), Dermatophagoides pteronyssinus (1,616 cases, 23.37%), and house dust (645 cases, 9.33%). The top three positive rates of food allergens were eggs (686 cases, 9.92%), milk (509 cases, 7.36%), and crabs (192 cases, 2.78%). The total positive rate of allergens was higher in men (46.99%) than in women (37.30%). Compared to 2 years before the COVID-19 epidemic, the rate of sensitization to indoor inhalant allergens increased, but outdoor inhalant allergens showed no significant change. The positive rates of milk and eggs peaked during the outbreak of COVID-19 (2020) then declined in 2021. The total positive rate of allergens was higher in males than females before and during the COVID-19 epidemic, but more allergens were different between males and females during the pandemic. Compared to middle-aged and older adults, the children and youth groups were more susceptible to allergic diseases, and they exhibited an increasing positive rate for most common allergens, especially indoor inhalant allergens, during the COVID-19 epidemic than before the pandemic. CONCLUSION: D. pteronyssinus and D. farinae are the most common allergens in South China. Under the background of normalization of epidemic prevention, indoor inhaled allergens should be first in the prevention and control of allergic diseases, and a combination of various indoor cleaning measures should be used to improve the efficiency of interventions.


Assuntos
COVID-19 , Hipersensibilidade , Masculino , Criança , Idoso , Adolescente , Pessoa de Meia-Idade , Humanos , Feminino , Adulto , Alérgenos , Pandemias , Prevalência , COVID-19/epidemiologia
7.
Pharmacol Res ; 190: 106733, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-36931541

RESUMO

Natural compounds are widely used to prevent and treat various diseases due to their antioxidant and anti-inflammatory effects. As a kind of promising natural compound, plant-derived exosome-like nanoparticles (PELNs) are extracted from multivesicular bodies of various edible plants, including vegetables, foods, and fruits, and mainly regulate the cellular immune response to pathogen attacks. Moreover, PELNs could remarkably interfere with the dynamic imbalance between pro-inflammatory and anti-inflammatory effects, facilitating to maintain the homeostasis of cellular immune microenvironment. PELNs may serve as a better alternative to animal-derived exosomes (ADEs) owing to their widespread sources, cost-effectiveness, and easy accessibility. PELNs can mediate interspecies communication by transferring various cargoes such as proteins, lipids, and nucleic acids from plant cells to mammalian cells. This review summarizes the biogenesis, composition, and classification of exosomes; the common separation, purification, and characterization methods of PELNs, the potential advantages of PELNs over ADEs; and the anti-inflammatory and immunomodulatory functions of PELNs in various diseases including colitis, cancer, and inflammation-associated metabolic diseases. Additionally, the future perspectives of PELNs and the challenges associated with their clinical application are discussed.


Assuntos
Exossomos , Nanopartículas , Neoplasias , Animais , Exossomos/metabolismo , Sistema Imunitário/metabolismo , Plantas , Neoplasias/metabolismo , Mamíferos , Microambiente Tumoral
8.
J Nanobiotechnology ; 21(1): 114, 2023 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-36978093

RESUMO

BACKGROUND: The past few years have witnessed a significant increase in research related to plant-derived extracellular vesicles (PDEVs) in biological and medical applications. Using biochemical technologies, multiple independent groups have demonstrated the important roles of PDEVs as potential mediators involved in cell-cell communication and the exchange of bio-information between species. Recently, several contents have been well identified in PDEVs, including nucleic acids, proteins, lipids, and other active substances. These cargoes carried by PDEVs could be transferred into recipient cells and remarkably influence their biological behaviors associated with human diseases, such as cancers and inflammatory diseases. This review summarizes the latest updates regarding PDEVs and focuses on its important role in nanomedicine applications, as well as the potential of PDEVs as drug delivery strategies to develop diagnostic and therapeutic agents for the clinical management of diseases, especially like cancers. CONCLUSION: Considering its unique advantages, especially high stability, intrinsic bioactivity and easy absorption, further elaboration on molecular mechanisms and biological factors driving the function of PDEVs will provide new horizons for the treatment of human disease.


Assuntos
Vesículas Extracelulares , Neoplasias , Humanos , Nanomedicina , Vesículas Extracelulares/metabolismo , Neoplasias/tratamento farmacológico , Neoplasias/metabolismo , Sistemas de Liberação de Medicamentos , Comunicação Celular
9.
J Nanobiotechnology ; 21(1): 204, 2023 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-37386404

RESUMO

Dihydroartemisinin (DHA), a natural product derived from the herbal medicine Artemisia annua, is recently used as a novel anti-cancer agent. However, some intrinsic disadvantages limit its potential for clinical management of cancer patients, such as poor water solubility and low bioavailability. Nowadays, the nanoscale drug delivery system emerges as a hopeful platform for improve the anti-cancer treatment. Accordingly, a metal-organic framework (MOF) based on zeolitic imidazolate framework-8 was designed and synthesized to carry DHA in the core (ZIF-DHA). Contrast with free DHA, these prepared ZIF-DHA nanoparticles (NPs) displayed preferable anti-tumor therapeutic activity in several ovarian cancer cells accompanied with suppressed production of cellular reactive oxygen species (ROS) and induced apoptotic cell death. 4D-FastDIA-based mass spectrometry technology indicated that down-regulated reactive oxygen species modulator 1 (ROMO1) might be regarded as potential therapeutic targets for ZIF-DHA NPs. Overexpression of ROMO1 in ovarian cancer cells significantly reversed the cellular ROS-generation induced by ZIF-DHA, as well as the pro-apoptosis effects. Taken together, our study elucidated and highlighted the potential of zeolitic imidazolate framework-8-based MOF to improve the activity of DHA to treat ovarian cancer. Our findings suggested that these prepared ZIF-DHA NPs could be an attractive therapeutic strategy for ovarian cancer.


Assuntos
Estruturas Metalorgânicas , Nanopartículas , Neoplasias Ovarianas , Humanos , Feminino , Espécies Reativas de Oxigênio , Neoplasias Ovarianas/tratamento farmacológico , Apoptose , Proteínas de Membrana , Proteínas Mitocondriais
10.
J Nanobiotechnology ; 21(1): 337, 2023 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-37735449

RESUMO

Staging lymph nodes (LN) is crucial in diagnosing and treating cancer metastasis. Biotechnologies for the specific localization of metastatic lymph nodes (MLNs) have attracted significant attention to efficiently define tumor metastases. Bioimaging modalities, particularly magnetic nanoparticles (MNPs) such as iron oxide nanoparticles, have emerged as promising tools in cancer bioimaging, with great potential for use in the preoperative and intraoperative tracking of MLNs. As radiation-free magnetic resonance imaging (MRI) probes, MNPs can serve as alternative MRI contrast agents, offering improved accuracy and biological safety for nodal staging in cancer patients. Although MNPs' application is still in its initial stages, exploring their underlying mechanisms can enhance the sensitivity and multifunctionality of lymph node mapping. This review focuses on the feasibility and current application status of MNPs for imaging metastatic nodules in preclinical and clinical development. Furthermore, exploring novel and promising MNP-based strategies with controllable characteristics could lead to a more precise treatment of metastatic cancer patients.


Assuntos
Nanopartículas de Magnetita , Neoplasias , Humanos , Neoplasias/diagnóstico por imagem , Fenômenos Físicos , Biotecnologia , Linfonodos/diagnóstico por imagem
11.
Sensors (Basel) ; 23(18)2023 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-37765794

RESUMO

In recent years, electric vehicles powered by lithium-ion batteries have developed rapidly, and the safety and reliability of lithium-ion batteries have been a paramount issue. Battery management systems are highly dependent on sensor measurements to ensure the proper functioning of lithium-ion batteries. Therefore, it is imperative to develop a suitable fault diagnosis scheme for battery sensors, to realize a diagnosis at an early stage. The main objective of this paper is to establish validated electrical and thermal models for batteries, and address a model-based fault diagnosis scheme for battery sensors. Descriptor proportional and derivate observer systems are applied for sensor diagnosis, based on electrical and thermal models of lithium-ion batteries, which can realize the real-time estimation of voltage sensor fault, current sensor fault, and temperature sensor fault. To verify the estimation effect of the proposed scheme, various types of faults are utilized for simulation experiments. Battery experimental data are used for battery modeling and observer-based fault diagnosis in battery sensors.

12.
J Environ Manage ; 342: 118235, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37270984

RESUMO

Countries around the world are increasingly turning towards developing digital economies to find better strategies for tackling the environmental pollution associated with economic growth while also pursuing high-quality economic conditions. This study aims to probe the link between coordinated regional digital economy development (RDEC) and air quality. A province-level RDEC indicator based on city-level data is developed, and air pollution is gauged by annual average PM2.5 concentrations. Furthermore, a spatial simultaneous equation model is employed to examine the causality further. The empirical results indicate that a bilateral causal relationship exists: RDEC improves air quality, and better air quality also facilitates RDEC. This relationship is influenced by spatial spillover effects. Specifically, air quality and RDEC of an area have a negative influence on the RDEC of neighboring regions, while they have a positive impact on neighboring areas' air quality. Further analysis suggests that green total factor productivity, advanced industrial structure, and regional entrepreneurship level can indirectly affect the contribution of RDEC to air quality. Additionally, the impact of air quality on RDEC may be realized through the increase in labor productivity, lower external environmental costs of regional economic development, and enhanced regional foreign economic exchange.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Poluentes Atmosféricos/análise , Desenvolvimento Econômico , Poluição do Ar/análise , Poluição Ambiental/análise , Cidades , China
13.
Zhong Nan Da Xue Xue Bao Yi Xue Ban ; 48(6): 809-820, 2023 Jun 28.
Artigo em Inglês, Zh | MEDLINE | ID: mdl-37587065

RESUMO

OBJECTIVES: Sepsis is a critical dysregulated host response with high mortality and current treatment is difficult to achieve optimal efficacy. Ozone therapy has been revealed to protect infection and inflammation-related diseases due to its role in antibiotic and immunoregulatory effect. Ozonated triglyceride is a key component of ozonated oil that is one of ozone therapy dosage form. However, the potential role of ozonated triglyceride in sepsis remains unclear. This study aims to explore the effect of ozonated triglyceride on septic mouse model and the molecular mechanism. METHODS: Intraperitoneal injection of lipopolysaccharide (LPS), cecal ligation and puncture (CLP) were applied to construct septic mouse model. The mouse serum was obtained for detection of cytokines, and lung tissues were collected for hematoxylin and eosin (HE) staining to evaluate the extent of lung injury in septic mouse with ozonated triglyceride treatment at different time and doses. The survival of septic mice was observed for 96 h and Kaplan-Meier analysis was used to analyze the survival rates. In addition, primary peritoneal macrophages and human acute monocytic-leukemia cell line (THP-1) were treated with inflammasome activators with or without ozonated triglyceride. The level of cytokines was detected by enzyme-linked immunosorbent assay (ELISA). The cleavage of caspase-1 and gasdermin-D (GSDMD) was detected by Western blotting. RESULTS: Ozonated triglyceride at different time and doses reduced the release of inflammasome-related cytokines [interleukin (IL)-1ß and IL-18] (all P<0.05) but not pro-inflammatory cytokines such as IL-6 and tumor necrosis factor-α (TNF-α) in septic mice (all P>0.05). Ozonated triglyceride significantly improved the survival rate of septic mice and reduced sepsis-induced lung injury (all P<0.05). Ozonated triglyceride significantly suppressed the canonical and non-canonical activation of NOD-like receptor family pyrin domain containing 3 (NLRP3) inflammasome (all P<0.05) but not affected absent in melanoma 2 (AIM2) and NLR family CARD domain-containing protein 4 (NLRC4) inflammasomes in vitro (all P>0.05). Ozonated triglyceride reduced the cleavage of caspase-1 and the downstream GSDMD. CONCLUSIONS: Ozonated triglyceride presents a protect effect on sepsis lethality via reducing cytokines release and sepsis-related organ injury. The mechanism is that ozonated triglyceride specifically suppresses the activation of NLRP3 inflammasome. Ozonated triglyceride is a promising candidate for sepsis treatment.


Assuntos
Lesão Pulmonar , Ozônio , Sepse , Animais , Humanos , Camundongos , Caspase 1 , Citocinas , Modelos Animais de Doenças , Inflamassomos , Proteína 3 que Contém Domínio de Pirina da Família NLR , Ozônio/farmacologia , Ozônio/uso terapêutico , Sepse/tratamento farmacológico
14.
Exp Dermatol ; 31(7): 986-992, 2022 07.
Artigo em Inglês | MEDLINE | ID: mdl-35524394

RESUMO

Due to a steady increase in the number of individuals suffering from alopecia, this condition has recently received increasing attention. Alopecia can be caused by various pathological, environmental or psychological factors, eventually resulting in abnormalities in hair follicle (HF) structures or HF regeneration disorders, especially dysregulated hair follicle stem cell (HFSC) behaviour. HFSC behaviour includes activation, proliferation and differentiation. Appropriate HFSC behaviour sustains a persistent hair cycle (HC). HFSC behaviour is mainly influenced by HFSC metabolism, ageing and the microenvironment. In this review, we summarize recent findings on how HFSC metabolism, ageing and the microenvironment give rise to hair growth disorders, as well as related genes and signalling pathways. Recent research on the application of stem cell-based hair tissue engineering and regenerative medicine to treat alopecia is also summarized. Determining how dysregulated HFSC behaviour underlies alopecia would be helpful in identifying potential therapeutic targets.


Assuntos
Alopecia , Folículo Piloso , Alopecia/patologia , Diferenciação Celular/fisiologia , Cabelo , Folículo Piloso/fisiologia , Humanos , Células-Tronco
15.
Inorg Chem ; 61(3): 1805-1815, 2022 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-35021010

RESUMO

Developing broadband cyan-emitting phosphors is an essential issue to achieve high-quality full-spectrum phosphor-converted white light-emitting diodes. Multisite cation regulation to modify the photoluminescence spectrum is a valid way to achieve broadband emission for phosphors. The Ba9Lu2Si6O24 lattice with various cation sites for activator ions is a preferred host for broadband emitting phosphors. The preferential crystallographic sites of Eu2+ in the Ba9Lu2Si6O24 lattice are identified based on the crystal field theory, crystal structure, and bond indices (such as NAC and SBOs) of the cations. Sr substitution in Ba9Lu2Si6O24/Eu2+ phosphor affects the location of Eu2+ activator ions, which is investigated via the first-principles density functional theory calculations, Rietveld refinement, and luminescence decay curves, and results in the modification of luminescence properties and thermal stability. The Sr-substituted (Ba0.8Sr0.2)9Lu2Si6O24/Eu2+ sample exhibits a broadband emission spectrum peaked at 471 and 518 nm with a large full width half maximum of 139 nm, covering blue-cyan-green regions, which can be an excellent candidate as broadband cyan-emitting phosphors for high-quality full-spectrum wLEDs.

16.
Angew Chem Int Ed Engl ; 61(51): e202210338, 2022 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-36266741

RESUMO

The first copper-catalyzed regiodivergent cyanoboration of internal allenes with B2 pin2 (bis(pinacolato)diboron) and NCTS (N-cyano-N-phenyl-p-toluenesulfonamide) derivatives is reported. The ß,γ- and α,ß-cyanoborylated products were synthesized with high regio- and stereo-selectivity. Computational studies revealed that nucleophilic addition of allylcopper or related intermediates on cyanation reagent is the regio- and stereo-determining step, while transmetalation with B2 pin2 is the rate-determining step. The nucleophilic addition step proceeds via inner-sphere mechanism in the CuI /P(o-tol)3 and CuI /Xantphos (P(o-tol)3 =tris(o-methylphenyl)phosphine, Xantphos=4,5-bis(diphenylphosphino)-9,9-dimethylxanthene) catalytic systems and via outer-sphere mechanism in the CuII /Xantphos catalytic system, respectively.

17.
Angew Chem Int Ed Engl ; 59(43): 18975-18979, 2020 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-32618077

RESUMO

An efficient copper-catalyzed regioselective C-H alkenylation and borylative alkylation of quinoline N-oxides with vinyl arenes in the presence of pinacol diborane has been developed. The reaction proceeds through the borylcupration of the vinyl arenes followed by nucleophilic attack of the resulting alkyl copper species to the quinoline N-oxides. Benzoquinone and KOt Bu were identified as the necessary additives at the second step of the reaction that are crucial for the success of the reaction. A wide range of C2-functionalizaed quinolines were obtained with good functional group tolerance, which may find utilities in pharmaceuticals and synthetic chemistry.

18.
J Org Chem ; 84(21): 13841-13857, 2019 11 01.
Artigo em Inglês | MEDLINE | ID: mdl-31566377

RESUMO

The general dehalogenation of alkyl halides with zinc using D2O or H2O as a deuterium or hydrogen donor has been developed. The method provides an efficient and economic protocol for deuterium-labeled derivatives with a wide substrate scope under mild reaction conditions. Mechanistic studies indicated that a radical process is involved for the formation of organozinc intermediates. The facile hydrolysis of the organozinc intermediates provides the driving force for this transformation.

19.
Inorg Chem ; 58(14): 9108-9117, 2019 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-31244085

RESUMO

Orange-yellow phosphors with extended broadband emission are highly desirable for warmer white-light-emitting diodes (WLED) with a higher color-rendering index. Targeted phosphors Ce3+-doped Lu3(MgxAl2-x)(Al3-xSix)O12 (x = 0, 0.25, 0.50, 0.75, and 1.00) were developed by chemical composition modification for luminescent tuning from green to orange-yellow with spectral broadening. The correlation between structure evolution and luminescent properties was elucidated by the local structure, fluorescence lifetime, and Eu3+ luminescence as a structural probe. The polyhedron distortion in the second-sphere coordination leads to the site differentiation and symmetry degradation of Ce3+ with the accommodation of (MgSi)6+ pairs, comprehensively resulting in the red shift (540 → 564 nm) and broadening in emission spectra. The WLED fabrication results demonstrate that the red shift and broadening in the emission of Lu3(MgxAl2-x)(Al3-xSix)O12:Ce3+ make it more suitable for the single-phosphor converted warm WLED.

20.
Inorg Chem ; 58(2): 1492-1500, 2019 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-30596246

RESUMO

High-quality white light-emitting diodes (w-LEDs) are mainly determined by conversion phosphors and the enhancement of cyan component that dominates the high color rendering index. New phosphors (Lu2M)(Al4Si)O12:Ce3+ (M = Mg, Ca, Sr and Ba), showing a cyan-green emission, have been achieved via the co-substitution of Lu3+-Al3+ by M2+-Si4+ pair in Lu3Al5O12:Ce3+ to compensate for the lack of cyan region and avoid using multiple phosphors. The excitation bands of (Lu2M)(Al4Si)O12:Ce3+ (M = Mg, Ca, Sr and Ba) show a red-shift from 434 to 445 nm which is attributed to the larger centroid shift and crystal field splitting. The enhanced structural rigidity associated with the accommodation of larger M2+ leads to a decreasing Stokes shift and the corresponding blue-shift (533 → 511 nm) in emission spectra, along with an improvement in thermal stability (keeping ∼93% at 150 °C). The cyan-green phosphor Lu2BaAl4SiO12:Ce3+ enables to fabricate a superhigh color rendering w-LED ( Ra = 96.6), verifying its superiority and application prospect in high-quality solid-state lightings.

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