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1.
RSC Adv ; 14(19): 12978-12982, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38655477

RESUMO

3d-Metal catalyzed borrowing hydrogen (BH) reactions represent powerful and environmentally friendly approaches for the direct coupling of alcohols with nitriles to assemble various important branched nitriles. The development of simple and efficient ligands is a crucial issue in this field. In this study, we designed a series of readily available N,N-bidentate ligands that demonstrated good efficiency in the Mn-catalyzed BH reaction of alcohols and nitrile derivatives, yielding the targeted nitriles in moderate to good yields. Remarkably, the mildness and practicality of this protocol were further demonstrated by the successful synthesis of anipamil via a two-cascade borrowing hydrogen procedure.

2.
Poult Sci ; 102(10): 102928, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37499610

RESUMO

Tianjin-monkey Chicken is a locally bred dual-purpose naked neck poultry with high tolerance to heat stress and poor reproductive ability. We aim to explore breeding-related genes to promote its growth, reproduction, meat, and egg performances. In this study, purebred, crossbred neck-naked and crossbred neck-feathered Tianjin-monkey Chickens (male = 5 and female = 5 in each group) were sampled for transcriptome analysis. Differential gene expression analysis was performed to identify candidate genes based on mRNA expression profiles. Functional enrichment analyses including GO, KEGG and GSEA analysis were conducted. Forty-five candidate breeding-related genes were identified, which were significantly enriched in 5 KEGG pathways and 37 GO terms. Some of the candidate genes were considered to be valuable in guiding breeding in the future, including SPRY3, CPXM2, FST, HDDC2, TLR1B, CYBB, and EHHADH.


Assuntos
Galinhas , Perfilação da Expressão Gênica , Animais , Feminino , Masculino , Galinhas/genética , Perfilação da Expressão Gênica/veterinária , Carne , Plumas , Reprodução/genética , Transcriptoma
3.
Cell Rep ; 40(3): 111077, 2022 07 19.
Artigo em Inglês | MEDLINE | ID: mdl-35858554

RESUMO

Redox-active metal ions are pivotal for rapid metabolism, proliferation, and aggression across cancer types, and this presents metal chelation as an attractive cancer cell-targeting strategy. Here, we identify a metal chelator, KS10076, as a potent anti-cancer drug candidate. A metal-bound KS10076 complex with redox potential for generating hydrogen peroxide and superoxide anions induces intracellular reactive oxygen species (ROS). The elevation of ROS by KS10076 promotes the destabilization of signal transducer and activator of transcription 3, removes aldehyde dehydrogenase isoform 1-positive cancer stem cells, and subsequently induces autophagic cell death. Bioinformatic analysis of KS10076 susceptibility in pan-cancer cells shows that KS10076 potentially targets cancer cells with increased mitochondrial function. Furthermore, patient-derived organoid models demonstrate that KS10076 efficiently represses cancer cells with active KRAS, and fluorouracil resistance, which suggests clinical advantages.


Assuntos
Morte Celular Autofágica , Fator de Transcrição STAT3 , Família Aldeído Desidrogenase 1 , Apoptose , Linhagem Celular Tumoral , Quelantes , Humanos , Células-Tronco Neoplásicas/metabolismo , Oxirredução , Espécies Reativas de Oxigênio/metabolismo , Fator de Transcrição STAT3/metabolismo , Superóxidos/metabolismo
4.
J Org Chem ; 87(12): 7864-7874, 2022 06 17.
Artigo em Inglês | MEDLINE | ID: mdl-35676758

RESUMO

A highly efficient Rh-catalyzed hydrogenation of functionalized olefins has been realized by a new family of highly rigid chiral ferrocenylphosphine-spiro phosphonamidite ligands. Excellent enantiocontrol (>99% ee in most cases) was achieved with a wide range of α-dehydroamino acid esters and α-enamides. This practicable catalytic system was further applied in the scalable synthesis of highly optically pure key intermediates of cinacalcet and d-phenylalanine.


Assuntos
Alcenos , Ródio , Alcenos/química , Catálise , Hidrogenação , Ligantes , Ródio/química , Estereoisomerismo
5.
Org Biomol Chem ; 19(44): 9746-9751, 2021 11 18.
Artigo em Inglês | MEDLINE | ID: mdl-34730165

RESUMO

The iridium/f-diaphos L1, L5 or L12 catalyzed asymmetric hydrogenation of 2-imidazolyl aryl/alkyl ketones to afford two enantiomers of the desired chiral alcohols with high conversions (up to 99% yield) and moderate to excellent enantioselectivities (61% - >99% ee) was realized for the first time. This protocol could be easily conducted on a gram-scale with a TON of 9700.

6.
J Phys Condens Matter ; 32(5): 055301, 2020 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-31600737

RESUMO

Using density functional theory and nonequilibrium Green's function method, the spin-dependent electronic transport properties of six transition metal porphyrin molecules (VP, CrP, MnP, FeP, CoP, and NiP), which are linked to gold electrodes through the thiolated ethynyl groups, are investigated. Two different linkage modes (beta linkage and meso linkage) of the substituted ethynyl groups on the porphyrin macrocycle are considered. The results show that the linkage mode of ethynyl groups plays an important role on the spin transport properties of the molecular junctions and the beta linkage is more favorable for the spin filtering efficiency of current than the meso linkages. The spin-up and spin-down energy levels show the different evolutions which is responsible for the difference of spin filtering efficiency between the two linkage modes. The computational results of total current show that the meso-linked molecular junctions have the better conductive performances than the beta-linked ones which may be caused by the different electronic transport paths.

7.
Inorg Chem ; 56(14): 8397-8407, 2017 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-28657296

RESUMO

To suppress concentration quenching and to improve charge-carrier injection/transport in the emission layer (EML) of phosphorescent organic light-emitting diodes (PhOLEDs), a facial homoleptic iridium(III) complex emitter with amorphous characteristics was designed and prepared in one step from a multifunctional spiro ligand containing spiro[fluorene-9,9'-xanthene] (SFX) unit. Single-crystal X-ray analysis of the resulting fac-Ir(SFXpy)3 complex revealed an enlarged Ir···Ir distance and negligible intermolecular π-π interactions between the spiro ligands. The emitter exhibits yellow emission and almost equal energy levels compared to the commercial phosphor iridium(III) bis(4-phenylthieno[3,2-c]pyridinato-N,C2')acetylacetonate (PO-01). Dry-processed devices using a common host, 4,4'-bis(N-carbazolyl)-1,1'-biphenyl, and the fac-Ir(SFXpy)3 emitter at a doping concentration of 15 wt % exhibited a peak performance of 46.2 cd A-1, 36.3 lm W-1, and 12.1% for the current efficiency (CE), power efficiency (PE), and external quantum efficiency (EQE), respectively. Compared to control devices using PO-01 as the dopant, the fac-Ir(SFXpy)3-based devices remained superior in the doping range between 8 and 15 wt %. The current densities went up with increasing doping concentration at the same driving voltage, while the roll-offs remain relatively low even at high doping levels. The superior performance of the new emitter-based devices was ascribed to key roles of the spiro ligand for suppressing aggregation and assisting charge-carrier injection/transport. Benefiting from the amorphous stability of the emitter, the wet-processed device also exhibited respectful CE, PE, and EQE of 32.2 cd A-1, 22.1 lm W-1, and 11.3%, respectively, while the EQE roll-off was as low as 1.7% at the luminance of 1000 cd m-2. The three-dimensional geometry and binary-conjugation features render SFX the ideal multifunctional module for suppressing concentration quenching, facilitating charge-carrier injection/transport, and improving the amorphous stability of iridium(III)-based phosphorescent emitters.

8.
ACS Appl Mater Interfaces ; 9(21): 17949-17960, 2017 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-28492078

RESUMO

Hydrothermal treatment of nickel acetate and phosphoric acid aqueous solution followed with a carbothermal reduction assisted phosphorization process using sucrose as the carbon source for the controlled synthesis of NixPy/C was successfully realized for the first time. The critical synthesis factors, including reduction temperature, phosphorus/nickel ratio, pH, and sucrose amount were systematically investigated. Remarkably, the carbon serves as a reducer and plays a determinative role in the transformation of Ni2P2O7 into Ni2P/C. The synthesis strategy is divided into four distinguishable stages: (1) hydrothermal preparation of Ni3(PO4)2·8H2O precursor for stabilizing P sources; (2) dimerization of Ni3(PO4)2·8H2O into more thermal stable Ni2P2O7 amorphous phase along with the generation of NiO; (3) carbothermal reduction and phosphidation of NiO into NixPy (0 ≤ y/x ≤ 0.5); and (4) further phosphidation of mixed-phase NixPy and carbothermal reduction of Ni2P2O7 into single-phase Ni2P. The resultant Ni2P, the highly active phase in electrocatalysis, was applied as counter electrode in a dye-sensitized solar cell (DSSC). The DSSC based on Ni2P with 10.4 wt.% carbon delivers a power conversion efficiency of 9.57%, superior to that of state-of-the-art Pt-based cell (8.12%). The abundant Niδ+ and Pδ- active sites and the metal-like conductivity account for its outstanding catalytic performance.

9.
Chem Asian J ; 12(8): 920-926, 2017 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-28213900

RESUMO

A novel perfluoro-1,4-phenylenyl 6H-indolo[2,3-b]quinoxaline derivative (TFBIQ) was designed and synthesized by using a C-H direct arylation method. The optoelectrical properties of the obtained TFBIQ were fully characterized by UV/Vis spectroscopy, photoluminescence spectroscopy, cyclic voltammetry, and a group of Alq3 -based green organic light-emitting diodes (OLEDs). Device A, which used 0.5 nm-thick TFBIQ as the interfacial modification layer, exhibited the five best advantages of device performance including a minimum turn-on voltage as low as 3.1 V, a maximum luminescence intensity as high as 26564 cd m-2 , a highest current density value of 348.9 mA cm-2 at a voltage of 11 V, the smallest efficiency roll-off, as well as the greatest power efficiency of 1.46 lm W-1 relative to all of the other tested devices with thicker TFBIQ and also 10 nm-thick MoO3 as hole-injection layers (HILs). As a promising candidate for an organic HIL material, the as-prepared TFBIQ exhibited a strong thickness effect on the performance of corresponding OLEDs. Furthermore, the theoretical calculated vertical ionization potential of the fluorinated TFBIQ suggests better anti-oxidation stability than that of the non-fluorinated structure.

10.
Int J Soc Psychiatry ; 62(2): 167-75, 2016 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-26631271

RESUMO

OBJECTIVE: It is imperative to know families' opinions about where patients should live after discharge from involuntary hospitalization in the era of community mental health. METHODS: Questionnaires were sent (March-May 2011) to 808 guardians of patients who were involuntarily hospitalized in Japan (response rate = 54.2%). The final sample size was 365 family members. Whether families wanted to live with the patient after discharge from the hospital was the primary outcome variable. The associations of the demographic characteristics of the patients and families with the outcome variable were tested using logistic regression analysis. RESULTS: Approximately, 19% of the family guardians wanted to live with the patient after discharge from the hospital. Their wish to cohabit was positively associated with being a female (vs male) patient, having three or more cohabitants in the home and having lived together before hospitalization, after adjusting for the other covariates. Long-term hospitalization (10 years or longer) and siblings were significantly associated with the families not wanting to cohabit, after adjusting for the other covariates. CONCLUSION: It is important to know families' opinions about patients' living situations after discharge from involuntary hospitalization to provide them with an effective support system.


Assuntos
Atitude , Relações Familiares , Família/psicologia , Transtornos Mentais/enfermagem , Idoso , Idoso de 80 Anos ou mais , Estudos Transversais , Feminino , Humanos , Japão , Tempo de Internação/estatística & dados numéricos , Modelos Logísticos , Masculino , Serviços de Saúde Mental , Pessoa de Meia-Idade , Assistência ao Paciente , Alta do Paciente , Características de Residência , Inquéritos e Questionários
11.
Guang Pu Xue Yu Guang Pu Fen Xi ; 36(4): 1085-9, 2016 Apr.
Artigo em Chinês | MEDLINE | ID: mdl-30052004

RESUMO

In this paper, with sulfuric acid as a catalyst and acetic acid as solution at the temperature of 120 ℃ and refluxing period for 24 hours, a sterically hindered bulky 9,9-diarylfluorene intermediate of [9-(4-anilino)-9-phenyl-fluorene] had been successfully designed and synthesized with Friedel-Crafts reaction. The molecular structure of this compound was characterized in detail with nuclear magnetic resonance hydrogen spectrum, mass spectrometry, infrared ray, and so on. Nuclear magnetic resonance hydrogen spectrum and infrared ray spectrum of the compound indicated that the characteristic functional group amino of the compound at 6.55 ppm, 3 481 and 3 385 cm-1, respectively. UV-visible and fluorescence spectra properties of 9-(4-anilino)-9-phenyl-fluorene were characterized and discussed preliminarily, respectively. The research results show that the 9-(4-anilino)-9-phenyl-fluorene with bulky steric hindrance effects has four main absorption peaks with wavelength of 243, 257, 298 and 311 nm in dichloromethane solution, respectively. Moreover, with the excitation wavelength of 308 nm, an emission spectrum curve was obtained with wavelength of 300~500 nm, which has the maximum emission peak of 328 nm with a slim peak at about 405 nm and a long tail to 500 nm. The long tail was probably attributed to the interaction of intermolecular hydrogen bonding from aniline. The appropriate scope of fluorescence emission (300~500 nm) make the compound overlap with the absorption spectra of the classic blue material Bis(3,5-difluoro-2-(2-pyridyl)phenyl-(2-carboxypyridyl)iridium (Ⅲ) (FIrpic) (300~500 nm). It is possible to obtain excellent host materials through proper molecular tailoring and prepare well for high performance light-emitting device. In order to further understand the photoelectric properties of the compound, we used acetonitrile as solvent and tetrabutylammonium hexafluorophosphate as electrolyte, and the electrochemical properties of the compound was characterized with cyclic voltammetry measurements.The onset of the reduction and oxidation potential of the compound are -0.759 and 0.898 V, and the corresponding HOMO and LUMO energy levels are -5.38 and -3.72 eV, which wolud be beneficial to holes and electrons injection/transportation and further modified to be excellent host materials. All of these data would provide a useful reference for further fabrication of organic semiconductor luminescent device with high performance.

12.
Psychiatry Clin Neurosci ; 69(9): 512-22, 2015 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-25801941

RESUMO

The aim of this review is to clarify the state of psychiatric admissions and discharges in Japan using statistical data collected from 1996 to 2012. We performed a secondary analysis of nationwide data on psychiatric hospitals, which are collected yearly by the Ministry of Health, Labour and Welfare. The latest national figures for indices defined in the 'Reform Vision of Mental Health and Welfare' (originally released in 2004) were 70.9% for 'discharge rate for newly admitted patients' and 23.3% for 'discharge rate for long-term patients', which have target rates of ≥76% and ≥29%, respectively. The national discharge rate for newly admitted patients was roughly on the increase, but appeared to reach a plateau in recent years. [Correction added on 17 July 2015, after first online publication: 'on the decline' has been corrected to 'on the increase' in the sentence above.] The national discharge rate for long-term patients was higher in 2012 than in 1999 and appeared to increase throughout the 2000s, although not enough to reach the target. Some improvements in the discharge rate for newly admitted patients indicated some progress in mental health reform, although problems should continue to be addressed in order to reach the targets. As for discharge rates of long-term admissions in local communities, some problems still remain to be solved in order to achieve the goals of the reform vision.


Assuntos
Inquéritos Epidemiológicos , Hospitais Psiquiátricos/estatística & dados numéricos , Pacientes Internados/estatística & dados numéricos , Hospitalização/estatística & dados numéricos , Humanos , Japão , Tempo de Internação/estatística & dados numéricos , Alta do Paciente/estatística & dados numéricos
13.
Dalton Trans ; 43(2): 599-608, 2014 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-24132227

RESUMO

To explore the photophysical properties of coordination compounds with enhanced two-photon absorption, two novel six-coordinated metal complexes (ML2, M = Cd(ii), Zn(ii)) from carbazole ß-diketone ligand (HL = 4,4,4-trifluoro-1-(9-butylcarbazole-3-yl)-1,3-butanedione) were prepared and fully characterized. Their crystal structures were determined by X-ray diffraction analysis. Both variable temperature (1)H NMR spectra and MALDI-TOF mass spectrometry proved that the coordination compounds exhibit good stability in solution. The results of time-dependent density functional theory (TD-DFT) calculations indicated that the complexation of the ligands with metal ion extends the electronic delocalization in the coordination compounds, leading to enhanced two-photon absorption. The photophysical properties for the coordination compounds were identified relying on both experimentally and theoretically studies. Finally, confocal microscopy and two-photon microscopy fluorescent imaging of HepG2 cells labeled with the Zn(ii) complexe revealed its potential applications as a biological fluorescent probe.


Assuntos
Cádmio/química , Hidrazinas/química , Imagem Molecular/métodos , Compostos Organometálicos/química , Fótons , Zinco/química , Absorção , Cristalografia por Raios X , Células Hep G2 , Humanos , Modelos Moleculares , Conformação Molecular , Teoria Quântica
14.
Asian J Psychiatr ; 6(1): 46-51, 2013 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-23380317

RESUMO

BACKGROUND: A combination of factors such as substance abuse problems, medication noncompliance, and insufficient insight are generally known to increase the risk of violent behavior. However, little is known regarding the psychological impact on caregivers who are traumatized by the violent behavior of a family member with schizophrenia. Therefore, we carried out an investigation to measure this impact. METHOD: A questionnaire was given to 116 caregivers of individuals with schizophrenia in family support groups in Seoul and Daegu, Korea. Their responses were then evaluated using the 22-item version of the Impact of Event Scale-Revised (IES-R), the 8-item short version of the Zarit Caregiver Burden Interview (ZBI-8), and the 15-item version of the Mental Illness and Disorder Understanding Scale (MIDUS). RESULTS: The mean (SD) IES-R score was 26.69 (17.83) (range, 1-84). Multiple regression analysis showed that the psychological impact of traumatic experiences was significantly associated with the following factors: medical non-adherence (P<0.01), living without the patient (P<0.01), and caregiver burden (P<0.05). CONCLUSION: Our results from the present study suggest that even when family caregivers live apart from the patient, they still experience the harmful psychological impact of trauma from the patient's violent behavior. The psychological impact continued as a result of the huge caregiver burden and the medication non-adherence of the family member with schizophrenia in spite of receiving long-term treatment and multiple hospitalizations. The present findings suggest the need for improved community-based service for preventive long-term care, including medication adherence, for outpatients with schizophrenia instead of multiple hospitalizations.


Assuntos
Cuidadores/psicologia , Esquizofrenia/enfermagem , Estresse Psicológico/psicologia , Violência/psicologia , Adulto , Família , Feminino , Humanos , Masculino , Adesão à Medicação , Pessoa de Meia-Idade , Características de Residência , Fatores de Risco , Esquizofrenia/complicações , Inquéritos e Questionários
15.
Chem Commun (Camb) ; 48(32): 3854-6, 2012 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-22406870

RESUMO

A 3-D platinum(II)-based spirometal complex has been designed and synthesized to suppress aggregation and excimer emission. A prototype phosphorescent organic light-emitting device exhibits the high-performance orange emission with an external quantum efficiency of up to 5.2%.

16.
Chem Commun (Camb) ; 47(46): 12467-9, 2011 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-22034622

RESUMO

A novel europium(III) ß-diketonate complex exhibiting bright two-photon-sensitized luminescence is synthesized and applied as a two-photon-sensitized luminescent probe to stain DNA in live cells.


Assuntos
Európio/química , Cetonas/química , Medições Luminescentes , Imagem Molecular/métodos , Compostos Organometálicos/química , Fótons , Linhagem Celular Tumoral , Humanos , Modelos Moleculares , Conformação Molecular , Compostos Organometálicos/síntese química
18.
Guang Pu Xue Yu Guang Pu Fen Xi ; 28(4): 883-6, 2008 Apr.
Artigo em Chinês | MEDLINE | ID: mdl-18619321

RESUMO

Two novel carbazole derivatives, 3-acetyl-9-n-hexylcarbazole (AHCZ) and 3, 6- diacetyl-9-n-hexylcarbazole (DHCZ) were synthesized through Friedel-Crafts reaction. The compounds were characterized by IR spectra, 1H NMR, MS and elemental analysis. UV-visible spectra of AHCZ and DHCZ were measured and compared with those of their precursors, 9-hexylcarbazole(HCZ) and carbazole(CZ). DHCZ and AHCZ exhibited strong absorption band, revealing the extent of pi conjugation in the system. TD-DFT method was performed to analyze the electronic absorption spectra of AHCZ and DHCZ, and the calculated excitation energies and oscillator strengths were compared with the experimental results.

19.
Artigo em Inglês | MEDLINE | ID: mdl-17271589

RESUMO

EEG-based brain computer interface (BCI) provides a completely new communication channel between human brain and computer. Classification of EEG signals is a difficult task, especially when the classification has to be preformed on a single-trial EEG to continuously control a device. Event related desynchronization (ERD) has proven to be induced on the contralateral sensorimotor area during imagination of a left or right hand movement. In this paper, we introduced a quantification of ERD, with which a lower classification error rate and a higher information transfer rate can be obtained. The performance was tested by the Graz dataset for BCI competition 2003.

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