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1.
Biotechnol Lett ; 42(10): 2049-2058, 2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-32500474

RESUMO

Cancer metastasis is the primary cause of death in patients diagnosed with colorectal cancer. Piperine, an active nontoxic ingredient in pepper, has potent anti-inflammatory and anti-cancer properties. However, little is known about the anti-migratory and anti-invasive effects of piperine on colorectal cancer. We demonstrated piperine inhibited the migration and invasion of colorectal cancer cells. Then, we found piperine reversed the biomarker expression of epithelial-to-mesenchymal transition (EMT), and suppressed the EMT regulator Snail. Furthermore, signal transducers and activators of transcription 3 (STAT3) was downregulated by piperine. Finally, STAT3 inhibitors were applied to observe the role of STAT3 in colorectal cancer migration, invasion and EMT. Collectively, piperine inhibits colorectal cancer migratory and invasive capacities through STAT3/Snail mediated EMT. Therefore, piperine could be applied as a possible therapeutic regimen for the prevention of colorectal cancer metastasis.

2.
Nanoscale ; 2020 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-32196063

RESUMO

Polymeric carbon nitrides (PCNs) are promising photocatalysts and electrocatalysts for water oxidation, as they are environmentally benign materials with an adjustable structure and facilely synthesized from inexpensive and abundant starting materials. In this minireview, we examine the state-of-the-art strategies for tailoring PCNs for efficient photocatalytic, electrocatalytic, and photoelectrochemical water oxidation, including heteroatom doping and interface engineering from band structure alignment (e.g., by coupling inorganic or organic semiconductors) to hybridization with nanoscale cocatalysts (e.g., nanosheets, nanoarrays, nanoparticles, and quantum dots) and sub-nanoscale cocatalysts (e.g., metallic molecular clusters and single-atom catalysts). Through establishing the structure-activity correlations, we aim to present a clear roadmap for providing insights into the design strategies, structure modification, and the improved catalytic performances of PCN-based materials in different catalytic water oxidation processes. For future guidance, we also propose some outlooks on the perspective and challenges of PCNs towards a better application in catalytic water oxidation.

3.
Adv Mater ; : e1905739, 2020 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-31957161

RESUMO

The structure-property engineering of phase-based materials for redox-reactive energy conversion and environmental decontamination nanosystems, which are crucial for achieving feasible and sustainable energy and environment treatment technology, is discussed. An exhaustive overview of redox reaction processes, including electrocatalysis, photocatalysis, and photoelectrocatalysis, is given. Through examples of applications of these redox reactions, how structural phase engineering (SPE) strategies can influence the catalytic activity, selectivity, and stability is constructively reviewed and discussed. As observed, to date, much progress has been made in SPE to improve catalytic redox reactions. However, a number of highly intriguing, unresolved issues remain to be discussed, including solar photon-to-exciton conversion efficiency, exciton dissociation into active reductive/oxidative electrons/holes, dual- and multiphase junctions, selective adsorption/desorption, performance stability, sustainability, etc. To conclude, key challenges and prospects with SPE-assisted redox reaction systems are highlighted, where further development for the advanced engineering of phase-based materials will accelerate the sustainable (active, reliable, and scalable) production of valuable chemicals and energy, as well as facilitate environmental treatment.

4.
Adv Mater ; 32(18): e1904037, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-31793723

RESUMO

Low-cost, nonprecious transition metal (TM) catalysts toward efficient water oxidation are of critical importance to future sustainable energy technologies. The advances in structure engineering of water oxidation catalysts (WOCs) with single TM centers as active sites, for example, single metallic molecular complexes (SMMCs), supported SMMCs, and single-atom catalysts (SACs) in recent reports are examined. The efforts made on these configurations in terms of design principle, advanced characterization, performances and theoretical studies, are critically reviewed. A clear roadmap with the correlations between the single-TM-site-based structures (coordination and geometric structure, TM species, support), and the catalytic performances in water oxidation is provided. The insights bridging SMMCs with SACs are also given. Finally, the challenges and opportunities in the single-TM-site catalysis are proposed.

5.
J Hazard Mater ; 389: 121881, 2020 05 05.
Artigo em Inglês | MEDLINE | ID: mdl-31852591

RESUMO

The biomass, bottlebrush flower, is exploited for the preparation of functionalized porous carbons by one-pot thermal activation using NaHCO3 and dicyandiamide. An intensified cross-linking effect among the precursors boosts pore (especially mesopore) formation in the pyrolysis process, producing N-doped porous carbons (NPCs) with a large specific surface area (SSA, up to 2025 m2 g-1). The biomass-derived carbon samples turn out to be highly effective in adsorption, and catalytic activation of peroxymonosulfate for degradation of aqueous phenol and p-hydroxybenzoic acid (HBA) in single and binary systems. The effects of N content, porous structure, and trace Ni species on the adsorptive and catalytic behavior of carbon are investigated. It is found that the porous structure plays a more critical role in adsorption than surface N functionality, while the contributions of various reactive species for phenol and HBA degradation are different.

6.
Dev Biol ; 456(1): 63-73, 2019 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-31419410

RESUMO

The organizer is an essential signaling center required for axial formation during vertebrate embryonic development. In the basal chordate amphioxus, the dorsal blastopore lip of the gastrula has been proposed to be homologous to the vertebrate organizer. Lefty is one of the first genes to be expressed in the organizer. The present results show that Lefty overexpression abolishes the organizer; the embryos were severely ventralized and posteriorized, and failed to develop anterior and dorsal structures. In Lefty knockouts the organizer is enlarged, and anterior and dorsal structures are expanded. Different from Lefty morphants in vertebrates, amphioxus Lefty mutants also exhibited left-right defects. Inhibition of Nodal with SB505124 partially rescued the effects of Lefty loss-of-function on morphology. In addition, while SB505124 treatment blocked Lefty expression in the cleavage stages of amphioxus embryos, activation of Nodal signaling with Activin protein induced ectopic Lefty expression at these stages. These results show that the interplay between Lefty and Nodal signaling plays an essential role in the specification of the amphioxus organizer and axes.

7.
Materials (Basel) ; 12(5)2019 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-30836696

RESUMO

This study analyzes the effects of shot peening on the crack initiation behavior under fretting loading by using a numerical method. The residual stress relaxation and the contact stress evolution are both considered. The crack initiation life is predicted by the critical plane Smith⁻Watson⁻Topper (SWT) model. Considering that the fretting contact region has a high stress gradient along the depth direction, the process volume approach is adopted to calculate the SWT parameters. The results show that the remaining residual stress after relaxation strongly affects crack initiation life. The remaining residual stress decreases with the increase of fatigue loading, and the effect of shot peening on the improvement of crack initiation life is more obvious under smaller fatigue loading. Furthermore, under smaller fatigue loading, the crack initiation life of specimens with high shot peening intensity is longer than that of specimens with low shot peening intensity. However, the opposite phenomenon appears when the fatigue loading is large enough.

8.
Adv Mater ; 30(39): e1803351, 2018 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-30059172

RESUMO

Quasi-1D cadmium chalcogenide quantum rods (QRs) are benchmark semiconductor materials that are combined with noble metals to constitute QR heterostructures for efficient photocatalysis. However, the high toxicity of cadmium and cost of noble metals are the main obstacles to their widespread use. Herein, a facile colloidal synthetic approach is reported that leads to the spontaneous formation of cadmium-free alloyed ZnSx Se1-x QRs from polydisperse ZnSe nanowires by alkylthiol etching. The obtained non-noble-metal ZnSx Se1-x QRs can not only be directly adopted as efficient photocatalysts for water oxidation, showing a striking oxygen evolution capability of 3000 µmol g-1 h-1 , but also be utilized to prepare QR-sensitized TiO2 photoanodes which present enhanced photo-electrochemical (PEC) activity. Density functional theory (DFT) simulations reveal that alloyed ZnSx Se1-x QRs have highly active Zn sites on the (100) surface and reduced energy barrier for oxygen evolution, which in turn, are beneficial to their outstanding photocatalytic and PEC activities.

9.
Chem Commun (Camb) ; 54(39): 4919-4922, 2018 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-29629462

RESUMO

We report a strategy for simultaneous cobalt removal and organic waste decomposition by using mesoporous hydroxyapatite nanoparticles wrapped in uniform carbon layers (HA@C). The in situ formation of CoOH+-HA@C due to ion exchange greatly improved the degradation efficiency by at least one order of magnitude compared to free Co2+.

10.
Nano Lett ; 18(2): 1373-1378, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29337565

RESUMO

Quantum mechanical effects of single particles can affect the collective plasmon behaviors substantially. In this work, the quantum control of plasmon excitation and propagation in graphene is demonstrated by adopting the variable quantum transmission of carriers at Heaviside potential steps as a tuning knob. First, the plasmon reflection is revealed to be tunable within a broad range by varying the ratio γ between the carrier energy and potential height, which originates from the quantum mechanical effect of carrier propagation at potential steps. Moreover, the plasmon excitation by free-space photos can be regulated from fully suppressed to fully launched in graphene potential wells also through adjusting γ, which defines the degrees of the carrier confinement in the potential wells. These discovered quantum plasmon effects offer a unified quantum-mechanical solution toward ultimate control of both plasmon launching and propagating, which are indispensable processes in building plasmon circuitry.

11.
J Colloid Interface Sci ; 514: 576-583, 2018 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-29294444

RESUMO

New photocatalytic materials for stable reduction and/or oxidization of water by harvesting a wider range of visible light are indispensable to achieve high practical efficiency in artificial photosynthesis. In this work, we prepared 2D WO3·H2O and WO3 nanosheets by a one-pot hydrothermal method and sequent calcination, focusing on the effects of crystal transformation on band structure and photocatalytic performance for photocatalytic water oxidation in the presence of electron acceptors (Ag+) under simulated solar light irradiation. The as-prepared WO3 nanosheets exhibit enhanced rate of photocatalytic water oxidation, which is 6.3 and 3.6 times higher than that of WO3·H2O nanosheets and commercial WO3, respectively. It is demonstrated that the releasing of water molecules in the crystal phase of tungstic acid results in transformation of the crystal phase from orthorhombic WO3·H2O to monoclinic WO3, significantly improving the activity of photocatalytic water oxidation in the presence of Ag+ because the shift-up of conduction band of WO3 matches well with the electrode potential of Ag+/Ag(s), leading to efficient separation of photoinduced electrons and holes in pure WO3 nanosheets.

12.
Phys Rev Lett ; 119(15): 156803, 2017 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-29077465

RESUMO

The interplays between different quasiparticles in solids lay the foundation for a wide spectrum of intriguing quantum effects, yet how the collective plasmon excitations affect the quantum transport of electrons remains largely unexplored. Here we provide the first demonstration that when the electron-plasmon coupling is introduced, the quantum coherence of electrons in graphene is substantially enhanced with the quantum coherence length almost tripled. We further develop a microscopic model to interpret the striking observations, emphasizing the vital role of the graphene plasmons in suppressing electron-electron dephasing. The novel and transformative concept of plasmon-enhanced quantum coherence sheds new insight into interquasiparticle interactions, and further extends a new dimension to exploit nontrivial quantum phenomena and devices in solid systems.

13.
Nanomaterials (Basel) ; 7(3)2017 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-28336897

RESUMO

Three-dimensional flower-like BiOI/BiOX (X = Br or Cl) hybrids were synthesized via a facile one-pot solvothermal approach. With systematic characterizations by X-ray diffraction (XRD), scanning electron microscopy (SEM), Transmission electron microscopy (TEM), the Brunauer-Emmett-Teller (BET)specific surface area, X-ray photoelectron spectroscopy (XPS), and the UV-Vis diffuse reflectance spectra (DRS), the BiOI/BiOCl composites showed a fluffy and porous 3-D architecture with a large specific surface area (SSA) and high capability for light absorption. Among all the BiOX (X = Cl, Br, I) and BiOI/BiOX (X = Cl or Br) composites, BiOI/BiOCl stands out as the most efficient photocatalyst under both visible and UV light irradiations for methyl orange (MO) oxidation. The reaction rate of MO degradation on BiOI/BiOCl was 2.1 times higher than that on pure BiOI under visible light. Moreover, BiOI/BiOCl exhibited enhanced water oxidation efficiency for O2 evolution which was 1.5 times higher than BiOI. The enhancement of photocatalytic activity could be attributed to the formation of a heterojunction between BiOI and BiOCl, with a nanoporous structure, a larger SSA, and a stronger light absorbance capacity especially in the visible-light region. The in situ electron paramagnetic resonance (EPR) revealed that BiOI/BiOCl composites could effectively evolve superoxide radicals and hydroxyl radicals for photodegradation, and the superoxide radicals are the dominant reactive species. The superb photocatalytic activity of BiOI/BiOCl could be utilized for the degradation of various industrial dyes under natural sunlight irradiation which is of high significance for the remediation of industrial wastewater in the future.

14.
Proc Natl Acad Sci U S A ; 114(14): 3684-3689, 2017 04 04.
Artigo em Inglês | MEDLINE | ID: mdl-28320954

RESUMO

Many bilaterally symmetrical animals develop genetically programmed left-right asymmetries. In vertebrates, this process is under the control of Nodal signaling, which is restricted to the left side by Nodal antagonists Cerberus and Lefty. Amphioxus, the earliest diverging chordate lineage, has profound left-right asymmetry as a larva. We show that Cerberus, Nodal, Lefty, and their target transcription factor Pitx are sequentially activated in amphioxus embryos. We then address their function by transcription activator-like effector nucleases (TALEN)-based knockout and heat-shock promoter (HSP)-driven overexpression. Knockout of Cerberus leads to ectopic right-sided expression of Nodal, Lefty, and Pitx, whereas overexpression of Cerberus represses their left-sided expression. Overexpression of Nodal in turn represses Cerberus and activates Lefty and Pitx ectopically on the right side. We also show Lefty represses Nodal, whereas Pitx activates Nodal These data combine in a model in which Cerberus determines whether the left-sided gene expression cassette is activated or repressed. These regulatory steps are essential for normal left-right asymmetry to develop, as when they are disrupted embryos may instead form two phenotypic left sides or two phenotypic right sides. Our study shows the regulatory cassette controlling left-right asymmetry was in place in the ancestor of amphioxus and vertebrates. This includes the Nodal inhibitors Cerberus and Lefty, both of which operate in feedback loops with Nodal and combine to establish asymmetric Pitx expression. Cerberus and Lefty are missing from most invertebrate lineages, marking this mechanism as an innovation in the lineage leading to modern chordates.


Assuntos
Padronização Corporal , Redes Reguladoras de Genes , Anfioxos/fisiologia , Animais , Regulação da Expressão Gênica no Desenvolvimento , Proteínas de Homeodomínio/metabolismo , Anfioxos/embriologia , Proteína Nodal/metabolismo , Proteínas Nucleares/metabolismo , Fatores de Transcrição Box Pareados/metabolismo , Transdução de Sinais
15.
J Colloid Interface Sci ; 493: 275-280, 2017 05 01.
Artigo em Inglês | MEDLINE | ID: mdl-28110062

RESUMO

Graphitic carbon nitride (g-C3N4) has been considered as a metal-free, cost-effective, eco-friendly and efficient catalyst for various photoelectrochemical applications. However, compared to conventional metal-based photocatalysts, its photocatalytic activity is still low because of the low mobility of carriers restricted by the polymer nature. Herein, a series of hybrids of g-C3N4 (GCN) and nanodiamonds (NDs) were synthesized using a solvothermal method. The photoelectrochemical performance and photocatalytic efficiency of the GCN/NDs were investigated by means of the generation of photocurrent and photodegradation of methylene blue (MB) solutions under UV-visible light irradiations. In this study, the sample of GCN/ND-33% derived from 0.1g GCN and 0.05g NDs displayed the highest photocatalytic activity and the strongest photocurrent density. The mechanism of enhanced photoelectrochemical and photocatalytic performances was also discussed.

16.
ACS Appl Mater Interfaces ; 8(51): 35203-35212, 2016 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-27977127

RESUMO

Direct water oxidation via photocatalysis is a four-electron and multiple-proton process which requires high extra energy input to produce free dioxygen gas, making it exacting, especially under visible light irradiation. To improve the oxygen evolution reaction rates (OERs) and utilize more visible light, flower-like cobalt hydroxide/oxide (Fw-Co(OH)2/Fw-Co3O4) photocatalysts were prepared and loaded onto graphitic carbon nitride (g-C3N4) by a facile coating method in this work. Influenced by the unique three-dimensional morphologies, the synthesized Fw-Co(OH)2 or Fw-Co3O4/g-C3N4 hybrids reveal favorable combination and synergism reflected by the modified photoelectric activities and the improved OER performances. Attributed to its prominent hydrotalcite structure, Fw-Co(OH)2 shows better cocatalytic activity for g-C3N4 modification compared with that of Fw-Co3O4. Specifically, 7 wt % Fw-Co(OH)2/g-C3N4 photocatalyst exhibits photocurrent density 4 times higher and OER performance 5 times better than pristine g-C3N4. This work unambiguously promotes the application of sustainable g-C3N4 in water oxidation.

17.
Chemosphere ; 159: 351-358, 2016 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-27318450

RESUMO

Novel uniform ellipsoid α-Mn2O3@α-MnO2 core/shell (McMs) nanocomposites were prepared via a hydrothermal process with a shape-control protocol followed by calcination at different temperatures. The properties of the composites were characterized by a number of techniques such as thermogravimetric analysis (TGA), X-ray diffraction (XRD), N2 adsorption, and scanning electron microscopy (SEM). The core/shell materials were much effective in heterogeneous oxone(®) activation to generate sulfate and hydroxyl radicals for degradation of aqueous phenol. The McMs composites demonstrated catalytic activity for 100% phenol decomposition in short duration varying between 20 and 120 min, much higher than that of homogeneous Mn(2+) system with 95% phenol degradation in 120 min. They also showed a higher activity than single-phase α-Mn2O3 or α-MnO2. The catalytic activity of phenol degradation depends on temperature, oxone(®) concentration, phenol concentration, and catalyst loading. The catalysts also showed a stable activity in several cycles. Kinetic study demonstrated that phenol degradation reactions follow a first order reaction on McMs catalysts giving activation energies at 32.1-68.8 kJ/mol. With the detection of radicals by electron paramagnetic resonance (EPR), the generation mechanism was proposed.


Assuntos
Compostos de Manganês/química , Nanopartículas/química , Óxidos/química , Fenol/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Adsorção , Catálise , Oxirredução , Purificação da Água/instrumentação , Difração de Raios X
18.
ACS Appl Mater Interfaces ; 8(11): 7184-93, 2016 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-26937827

RESUMO

Heteroatom (nitrogen and sulfur)-codoped porous carbons (N-S-PCs) with high surface areas and hierarchically porous structures were successfully synthesized via direct pyrolysis of a mixture of glucose, sodium bicarbonate, and thiourea. The resulting N-S-PCs exhibit excellent adsorption abilities and are highly efficient for potassium persulfate activation when employed as catalysts for the oxidative degradation of sulfachloropyridazine (SCP) solutions. The adsorption capacities of N-S-PC-2 (which contains 4.51 atom % nitrogen and 0.22 atom % sulfur and exhibits SBET of 1608 m(2) g(-1)) are 73, 7, and 3 times higher than those of graphene oxide, reduced graphene oxide, and commercial single-walled carbon nanotube, respectively. For oxidation, the reaction rate constant of N-S-PC-2 is 0.28 min(-1). This approach not only contributes to the large-scale production and application of high-quality catalysts in water remediation but also provides an innovative strategy for the production of heteroatom-doped PCs for energy applications.


Assuntos
Carbono/química , Nitrogênio/química , Sulfanilamidas/química , Enxofre/química , Oxirredução , Porosidade
19.
Materials (Basel) ; 8(10): 7094-7105, 2015 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-28793621

RESUMO

Residual compressive stress can improve fretting fatigue strength. In this paper, the effects of residual stress on fretting fatigue of Al 2024-T351 alloy specimens are studied using a numerical approach. The extended finite element method combined with the cyclic cohesive zone model is adopted to model fretting fatigue crack growth behavior. It is shown that residual stress changes the fretting fatigue crack growth path and enhances fretting fatigue life. Crack initiation angle, depth of knee point, crack initiation life, crack propagation life and total life are greater for specimens with residual stress compared to specimens without residual stress. The effects of residual stress are more remarkable for specimens with a high intensity of residual stress. However, the effects of residual stress reduce at a high bulk load level.

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