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1.
J Am Chem Soc ; 140(37): 11716-11725, 2018 09 19.
Artigo em Inglês | MEDLINE | ID: mdl-30153411

RESUMO

All-inorganic lead halide perovskites demonstrate improved thermal stability over the organic-inorganic halide perovskites, but the cubic α-CsPbI3 with the most appropriate bandgap for light harvesting is not structurally stable at room temperature and spontaneously transforms into the undesired orthorhombic δ-CsPbI3. Here, we present a new member of black-phase thin films of all-inorganic perovskites for high-efficiency photovoltaics, the orthorhombic γ-CsPbI3 thin films with intrinsic thermodynamic stability and ideal electronic structure. Exempt from introducing organic ligands or incorporating mixed cations/anions into the crystal lattice, we stabilize the γ-CsPbI3 thin films by a simple solution process in which a small amount of H2O manipulates the size-dependent phase formation through a proton transfer reaction. Theoretical calculations coupled with experiments show that γ-CsPbI3 with a lower surface free energy becomes thermodynamically preferred over δ-CsPbI3 at surface areas greater than 8600 m2/mol and exhibits comparable optoelectronic properties to α-CsPbI3. Consequently, γ-CsPbI3-based solar cells display a highly reproducible efficiency of 11.3%, among the highest records for CsPbI3 thin-film solar cells, with robust stability in ambient atmosphere for months and continuous operating conditions for hours. Our study provides a novel and fundamental perspective to overcome the Achilles' heel of the inorganic lead iodide perovskite and opens it up for high-performance optoelectronic devices.

2.
Nanoscale ; 9(43): 16826-16835, 2017 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-29072743

RESUMO

To increase the volumetric and gravimetric capacitances of supercapacitors, a new class of electrode materials with high electrochemical activity and favorable structures is extremely desired. In this work, a hollow novel nitrogen-doped 3D elastic single-walled carbon nanotube sponge (NSCS) which is ultra lightweight with the lowest density of 0.8 mg cm-3, and has a high open surface structure for electrolyte accessibility and excellent compressible properties as the electrode scaffold has been successfully fabricated by the pyrolysis method which could produce the carbon nanotube sponge easily on a large scale without high-cost and time-consuming processes. Moreover, a NiCo2O4 nanosheet supported on the NSCS has been successfully fabricated. The highest volumetric and gravimetric capacitance of this electrode is 790 F cm-3 at 1.43 g cm-3 and 1618 F g-1 at 0.54 g cm-3 with excellent cycling stability. The density of NiCo2O4/NSCS electrode was adjusted by mechanical compression and the most favorable density of the film for both high volumetric and gravimetric capacitances obtained was 1.21 g cm-3. The thick NiCo2O4/NSCS film of 72 µm has been fabricated at this favorable density, presenting both high volumetric and gravimetric capacitances of 597 F cm-3 and 1074 F g-1 at 1 A g-1, respectively, indicating that the structure of the NSCS is extremely feasible for obtaining a thick film electrode with excellent volumetric and gravimetric capacitances. Furthermore, an asymmetric supercapacitor of NiCo2O4/NSCS//NGN/CNTs was fabricated, exhibiting a high gravimetric energy density of 47.65 W h kg-1 at 536 W kg-1 and a volumetric energy density of 33.44 W h L-1 at 376.16 W L-1.

3.
Inorg Chem ; 56(15): 9291-9302, 2017 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-28749133

RESUMO

A series of two-dimensional (2D) hybrid organic-inorganic perovskite (HOIP) crystals, based on acene alkylamine cations (i.e., phenylmethylammonium (PMA), 2-phenylethylammonium (PEA), 1-(2-naphthyl)methanammonium (NMA), and 2-(2-naphthyl)ethanammonium (NEA)) and lead(II) halide (i.e., PbX42-, X = Cl, Br, and I) frameworks, and their corresponding thin films were fabricated and examined for structure-property relationship. Several new or redetermined crystal structures are reported, including those for (NEA)2PbI4, (NEA)2PbBr4, (NMA)2PbBr4, (PMA)2PbBr4, and (PEA)2PbI4. Non-centrosymmetric structures from among these 2D HOIPs were confirmed by piezoresponse force microscopy-especially noteworthy is the structure of (PMA)2PbBr4, which was previously reported as centrosymmetric. Examination of the impact of organic cation and inorganic layer choice on the exciton absorption/emission properties, among the set of compounds considered, reveals that perovskite layer distortion (i.e., Pb-I-Pb bond angle between adjacent PbI6 octahedra) has a more global effect on the exciton properties than octahedral distortion (i.e., variation of I-Pb-I bond angles and discrepancy among Pb-I bond lengths within each PbI6 octahedron). In addition to the characteristic sharp exciton emission for each perovskite, (PMA)2PbCl4, (PEA)2PbCl4, (NMA)2PbCl4, and (PMA)2PbBr4 exhibit separate, broad "white" emission in the long wavelength range. Piezoelectric compounds identified from these 2D HOIPs may be considered for future piezoresponse-type energy or electronic applications.

4.
ACS Nano ; 9(10): 10252-7, 2015 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-26390200

RESUMO

A core/shell stretchable conductive composite of a few-walled carbon nanotube network coated on a poly(m-phenylene isophthalamide) fiber (FWNT/PMIA) was fabricated by a dip-coating method and an annealing process that greatly enhanced interactions between the FWNT network and PMIA core as well as within the FWNT network. The first strain-conductivity test of the as-prepared FWNT/PMIA fiber showed a stretching-induced alignment of nanotubes in the shell during the deformation process and a good conductivity stability with a slight conductivity drop from 109.63 S/cm to 98.74 S/cm (Δσ/σ0 = 10%) at a strain of ∼150% (2.5 times the original length). More importantly, after the first stretching process, the fiber can be recovered with a slight increase in length but a greatly improved conductivity of 167.41 S/cm through an additional annealing treatment. The recovered fiber displays a similarly superb conductivity stability against stretching, with a decrease of only ∼13 S/cm to 154.49 S/cm (Δσ/σ0 = 8%) at a strain of ∼150%. We believe that this conductivity stability came from the formation and maintaining of aligned nanotube structures during the stretching process, which ensures the good tube-tube contacts and the elongation of the FWNT network without losing its conductivity. Such stable conductivity in stretchable fibers will be important for applications in stretchable electronics.

5.
Cancer Res ; 64(12): 4209-17, 2004 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-15205333

RESUMO

Lysophosphatidic acid (LPA) is present at high concentrations in ascites and plasma of ovarian cancer patients. Studies conducted in experimental models demonstrate that LPA promotes ovarian cancer invasion/metastasis by up-regulating protease expression, elevating protease activity, and enhancing angiogenic factor expression. In this study, we investigated the effect of LPA on ovarian cancer migration, an essential component of cancer cell invasion. LPA stimulates both chemotaxis and chemokinesis of ovarian cancer cells and LPA-stimulated cell migration is G(I) dependent. Moreover, constitutively active H-Ras enhances ovarian cancer cell migration, whereas dominant negative H-Ras blocks LPA-stimulated cell migration, suggesting that Ras works downstream of G(i) to mediate LPA-stimulated cell migration. Interestingly, H-Ras mutants that specifically activate Raf-1, Ral-GDS, or phosphatidylinositol 3'-kinase are unable to significantly enhance ovarian cancer cell migration, suggesting that a Ras downstream effector distinct from Raf-1, Ral-GDS, and phosphatidylinositol 3'-kinase is responsible for LPA-stimulated cell migration. In this article, we demonstrate that LPA activates mitogen-activated protein kinase kinase 1 (MEKK1) in a G(i)-Ras-dependent manner and that MEKK1 activity is essential for LPA-stimulated ovarian cancer cell migration. Inhibitors that block MEKK1 downstream pathways, including MEK1/2, MKK4/7, and nuclear factor-kappa B pathways, do not significantly alter LPA-stimulated cell migration. Instead, LPA induces the redistribution of focal adhesion kinase to focal contact regions of the cytoplasm membrane, and this event is abolished by pertussis toxin, dominant negative H-Ras, or dominant negative MEKK1. Our studies thus suggest that the G(i)-Ras-MEKK1 signaling pathway mediates LPA-stimulated ovarian cancer cell migration by facilitating focal adhesion kinase redistribution to focal contacts.


Assuntos
Movimento Celular/efeitos dos fármacos , Lisofosfolipídeos/farmacologia , MAP Quinase Quinase Quinase 1 , MAP Quinase Quinase Quinases/fisiologia , Neoplasias Ovarianas/enzimologia , Neoplasias Ovarianas/patologia , Proteínas ras/fisiologia , Movimento Celular/fisiologia , Feminino , Quinase 1 de Adesão Focal , Proteína-Tirosina Quinases de Adesão Focal , Adesões Focais/enzimologia , Fase G1/fisiologia , Humanos , Sistema de Sinalização das MAP Quinases/efeitos dos fármacos , Sistema de Sinalização das MAP Quinases/fisiologia , Proteínas Tirosina Quinases/metabolismo , Estimulação Química
6.
J Immunol ; 172(11): 7002-7, 2004 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-15153521

RESUMO

TL1A, a recently described TNF-like cytokine that interacts with DR3, costimulates T cells and augments anti-CD3 plus anti-CD28 IFN-gamma production. In the current study we show that TL1A or an agonistic anti-DR3 mAb synergize with IL-12/IL-18 to augment IFN-gamma production in human peripheral blood T cells and NK cells. TL1A also enhanced IFN-gamma production by IL-12/IL-18 stimulated CD56(+) T cells. When expressed as fold change, the synergistic effect of TL1A on cytokine-induced IFN-gamma production was more pronounced on CD4(+) and CD8(+) T cells than on CD56(+) T cells or NK cells. Intracellular cytokine staining showed that TL1A significantly enhanced both the percentage and the mean fluorescence intensity of IFN-gamma-producing T cells in response to IL-12/IL-18. The combination of IL-12 and IL-18 markedly up-regulated DR3 expression in NK cells, whereas it had minimal effect in T cells. Our data suggest that TL1A/DR3 pathway plays an important role in the augmentation of cytokine-induced IFN-gamma production in T cells and that DR3 expression is differentially regulated by IL-12/IL-18 in T cells and NK cells.


Assuntos
Interferon gama/biossíntese , Interleucina-12/farmacologia , Interleucina-18/farmacologia , Células Matadoras Naturais/efeitos dos fármacos , Linfócitos T/efeitos dos fármacos , Fator de Necrose Tumoral alfa/farmacologia , Antígeno CD56/análise , Sinergismo Farmacológico , Antígeno HLA-DR3/fisiologia , Humanos , Células Matadoras Naturais/imunologia , Linfócitos T/imunologia , Membro 15 da Superfamília de Ligantes de Fatores de Necrose Tumoral
7.
J Biol Chem ; 277(50): 48379-85, 2002 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-12377770

RESUMO

We reported previously that down-regulating or functionally blocking alphav integrins inhibits endogenous p38 mitogen-activated protein kinase (MAPK) activity and urokinase plasminogen activator (uPA) expression in invasive MDA-MB-231 breast cancer cells whereas engaging alphav integrins with vitronectin activates p38 MAPK and up-regulates uPA expression (Chen, J., Baskerville, C., Han, Q., Pan, Z., and Huang, S. (2001) J. Biol. Chem. 276, 47901-47905). Currently, it is not clear what upstream and downstream signaling molecules of p38 MAPK mediate alphav integrin-mediated uPA up-regulation. In the present study, we found that alphav integrin ligation activated small GTPase Rac1 preferentially, and dominant negative Rac1 inhibited alphav integrin-mediated p38 MAPK activation. Using constitutively active MAPK kinases, we found that both constitutively active MKK3 and MKK6 mutants were able to activate p38 MAPK and up-regulate uPA expression, but only dominant negative MKK3 blocked alphav integrin-mediated p38 MAPK activation and uPA up-regulation. These results suggest that MKK3, rather than MKK6, mediates alphav integrin-induced p38 MAPK activation. Among the potential downstream effectors of p38 MAPK, we found that only MAPK-activated protein kinase 2 affects alphav integrin-mediated uPA up-regulation significantly. Finally, using beta-globin reporter gene constructs containing uPA mRNA 3'-untranslated region (UTR) and adenosine/uridine-rich elements-deleted 3'-UTR, we demonstrated that p38 MAPK/MAPK-activated protein kinase 2 signaling pathway regulated uPA mRNA stability through a mechanism involving the adenosine/uridine-rich elements sequence in 3'-UTR of uPA mRNA.


Assuntos
Neoplasias da Mama/enzimologia , Quinases de Proteína Quinase Ativadas por Mitógeno/metabolismo , Proteínas Quinases Ativadas por Mitógeno/metabolismo , Proteínas Serina-Treonina Quinases/metabolismo , Proteínas Tirosina Quinases/metabolismo , RNA Mensageiro/genética , Ativador de Plasminogênio Tipo Uroquinase/genética , Proteínas rac1 de Ligação ao GTP/metabolismo , Regiões 3' não Traduzidas , Sequência de Bases , Neoplasias da Mama/patologia , Primers do DNA , Humanos , Peptídeos e Proteínas de Sinalização Intracelular , MAP Quinase Quinase 3 , Invasividade Neoplásica , Células Tumorais Cultivadas , Regulação para Cima , Proteínas Quinases p38 Ativadas por Mitógeno
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