Delicate elaboration of the nanostructures of multimetal catalytic materials with well-defined shapes and compositions to reveal their potential use as heterogeneous nanocatalysts for organic synthetic reactions with the combined merits of heterogeneous and homogeneous catalysis is both scientifically and technologically important, but this type of investigation has remained rarely pursued. In this work, we demonstrated a facile hydrothermal approach toward the one-pot shape-selective syntheses of Pd−Rh nanocrystals with tunable compositions and morphologies, including hollow nanocubes (NCs), nanoicosahedrons (NIs), and nanotruncated octahedrons (NTOs), using poly(vinylpyrrolidone) as both reductant and capping agent and halide anions (Br − /I − ) as shape control agents. The formation of Pd−Rh hollow NCs was induced by an iodine adsorbate-induced reconstruction mechanism with KI, whereas the formation of Pd−Rh NIs and NTOs were realized by controlling the selective nucleation of twinned seeds or single crystal seeds and their relative growth rates along different facets (e.g., ( 111) and (100) facets) through finely adjusting the Pd/Rh ratio and the amount of KBr added in the absence of KI. Due to the great significance of Pd-catalyzed organic reactions, the catalytic performances of Pd−Rh nanocrystals for Suzuki cross-coupling reactions with different reactants were evaluated. The measured turnover frequencies (TOFs) suggested that Pd−Rh hollow NCs held considerably enhanced catalytic activities (at least 3 times) than other Pd-based solid nanocrystals including Pd−Rh NIs, Pd−Rh NTOs, Pd−Rh NCs, Pd NCs, and commercial Pd/C, with iodobenzene as the reactant. In addition, even for more inert reactants such as bromobenzene or 4-bromotoluene, the catalytic activities of Pd−Rh hollow NCs were still impressive (showing similar TOFs to those of other shapes for reactions with iodobenzene as the reactant), indicating the promising application of Pd-based nanocatalysts for other powerful Pd-catalyzed organic synthesis reactions. Meanwhile, Pd-based solid NCs, enclosed with (100) facets only, showed better catalytic performance than NIs as well as NTOs, which had a larger fraction of (111) facets other than (100) ones, further suggesting that morphology differences were vitally significant to tune the catalytic performances of bimetallic nanocatalysts.
Multidimensional fabrication of metal-organic frameworks (MOFs) into multilevel channel integrated devices are in high demanded for Li-S separators.S uchs eparators have advantages in pore-engineering that might fulfill requirements such as intercepting the diffusing polysulfides and improving the Li + /electrolyte transfer in Li-S batteries.H owever,most reported works focus on the roles of MOFs as ionic sieves for polysulfides while offering limited investigation on the tuning of Li + transfer across the separators.Ap hotoinduced heat-assisted processing strategy is proposed to fabricate MOFs into multidimensional devices (e.g., hollow/ Janus fibers,d ouble-or triple-layer membranes). Fort he first time,at riple-layer separator with stepped-channels has been designed and demonstrated as ap owerful separator with outstanding specific capacity (1365.0 mAh g À1 )a nd cycling performance (0.03 %fading per cycle from 100 th to 700 th cycle), which is superior to single/double-layer and commercial separators.T he findings may expedite the development of MOF-based membranes and extend the scope of MOFs in energy-storage technologies.
Atomic-scale construction and high-throughput screening of robust multicomponent nanocatalysts with tunable well-defined surface structures and associated active sites for ethanol electro-oxidation reaction (EOR) in high activity and selectivity, referring to C−C bond cleavage and full oxidation of ethanol as a clean and sustainable energy source, has remained a great challenge. Herein, we demonstrate a powerful conceptual approach to design, synthesize and optimize single-crystalline Pt−Pd−Rh nanocrystals of altered shapes and compositions for enhanced EOR performance, based on combined density functional theory (DFT) calculations and experiment study. (111)-terminated Pt−Pd−Rh nano-truncated-octahedrons (NTOs) and (100)-terminated Pt−Pd−Rh nanocubes (NCs) with varied-compositions were prepared by regulating the reduction tendency of metal precursors in a facile hydrothermal method. Aided by DFT calculations, Pt3PdRh NTOs, PtPdRh NTO, and 8.8 nm PtPdRh NCs-200 were screened to be the best performing catalysts with the highest EOR activity (five times as much as that of commercial Pt black) at 0.5 V vs. NHE. Amongst these catalysts, PtPdRh NTOs exhibited the highest selectivity to CO2 at 0.5 V and the noteworthy capability to fully oxidize ethanol at extremely low potential (0.35 V); 8.8 nm PtPdRh NCs-200 possessed the best durability. Morphology and surface composition correlated to the synergistic effect of three metals were verified to affect the EOR performance of well-shaped Pt−Pd−Rh nanocrystals. Combined with in situ FTIR, it was deduced that appropriate surface composition and exposed facets were the key factors to the promoted capability in the cleavage of C−C bond down to low potential. Through adjusting surface composition and morphology of Pt−Pd−Rh nanocrystals with homogeneous element distribution, enhanced EOR performance was achieved in light of DFT simulations of the two elementary reactions (i.e., breakdown of C−C bond, and oxidation of COad). This work has offered an effective and useful strategy to promote the reactivity of multicomponent heterogeneous nanocatalysts with optimized compositions and surface structures for many industrial catalytic processes.
Brueckner-Hartree-Fock theory allows to derive the G-matrix as an effective interaction between nucleons in the nuclear medium. It depends on the center of mass momentum P of the two particles and on the two relative momenta q and q ′ before and after the scattering process. In the evaluation of the total energy per particle in nuclear matter usually the angle averaged center of mass momentum approximation has been used. We derive in detail the exact expressions of the angular integrations of the momentum P within relativistic Brueckner-Hartree-Fock (RBHF) theory, especially for the case of asymmetric nuclear matter. In order to assess the reliability of the conventional average momentum approximation for the binding energy, the saturation properties of symmetric and asymmetric nuclear matter are systematically investigated based on the realistic Bonn nucleon-nucleon potential. It is found that the exact treatment of the center of mass momentum leads to non-negligible contributions to the higher order physical quantities. The correlation between the symmetry energy E sym , the slope parameter L, and the curvature K sym of the symmetry energy are investigated. The results of our RBHF calculations for the bulk parameters characterizing the equation of state are compared with recent constraints extracted from giant monopole resonance and isospin diffusion experiments.
Background The association between RLS and migraine is still debated. The aim of this study is to investigate the prevalence and grade of RLS in Chinese patients with migraine and to evaluate the relationship between RLS and migraine. Methods A multi-center case-control study of contrast-enhanced transcranial Doppler was conducted in 931 consecutive patients with migraine (240 of 931 had migraine with aura and 691 of 931 were in the migraine without aura group) and 282 were healthy adults. Clinical trial no. NCT02425696. Results The prevalence of RLS was 63.8% and 39.9% in the migraine with aura group (MA+) and migraine without aura group (MA-), respectively, significantly higher than that of the healthy group (29.4%, p < 0.001; p < 0.001). The positive rate of large RLS in the MA+ group and MA- group was 32.1% and 16.5%, respectively, significantly higher than healthy group (6.4%, p < 0.001; p < 0.001). There was no difference among groups in terms of positive rate of permanent RLS ( p = 0.704). Conclusion This multi-centre case-control study suggested that there is an association between RLS and migraine with and without aura, especially when the shunt is large.
Background/Aims: Epigallocatechin-3-gallate (EGCG), a major catechin found in green tea, has been shown to prevent cardiovascular diseases. Previously, Matrix metalloproteinase-9 (MMP-9), monocyte chemotactic protein-1 (MCP-1) and toll-like receptor 4 (TLR4) were confirmed to play an important role in atherosclerosis and plaque instability. Both TLR4 and its negative regulator, Toll-interacting protein (Tollip), could be mediated by EGCG. The present study aimed to examine the effect of physiological concentration of EGCG (1 µM) on the expression of MMP-9 and MCP-1 in lipopolysaccharide (LPS)-induced macrophages and the potential mechanisms underlying its actions. Methods: The RAW264.7 cell line was used. Western blot was used to determine MCP-1, TLR4, Tollip, Mitogen-activated protein kinase (MAPK) and Nuclear factor-κB (NF-κB) protein expression. MMP-9 activity was assayed by gelatine zymography. The mRNA expression of MMP-9 and MCP-1 was measured by realtime polymerase chain reaction (RT-PCR). Results: EGCG (1 µM) significantly suppressed the expression of MMP-9 and MCP-1 and inhibited MAPK and NF-κB in LPS-induced macrophages but was blocked by Tollip silencing. The expression of LPS-induced MMP-9 and MCP-1 and the phosphorylation of the ERK1/2, P38 and NF-κB pathway proteins decreased after TLR4 siRNA treatment. Furthermore, EGCG mediated TLR4 and Tollip expression through binding to 67-kDa laminin receptor (67LR). Conclusion: The results of our study suggested that EGCG (1 µM) suppresses the TLR4/MAPK/NF-κB signalling pathway, decreases the expression of the plaque instability-mediating cytokines MMP-9 and MCP-1, and might prove to be effective in stabilizing atherosclerotic plaque.
Long noncoding RNAs (lncRNAs) have been increasingly considered to play an important role in the pathological process of various cardiovascular diseases, which often bind to the proximal promoters of the protein-coding gene to regulate the protein expression. However, the functions and mechanisms of lncRNAs in cardiomyocytes have not been fully elucidated. High-throughput RNA sequencing was performed to identify the differently expressed lncRNAs and messenger RNAs (mRNAs) between acute myocardial infarction (AMI) rats and healthy controls. One novel lncRNA FGF9-associated factor (termed FAF) and mRNAs in AMI rats were verified by bioinformatics, real-time polymerase chain reaction or western blot. Moreover, RNA fluorescence in situ hybridization was performed to determine the location of lncRNA. Subsequently, a series of in vitro assays were used to observe the functions of lncRNA FAF in cardiomyocytes. The expression of lncRNA FAF and FGF9 were remarkably decreased in ischemiahypoxia cardiomyocytes and heart tissues of AMI rats. Overexpression of FAF could significantly inhibit cardiomyocytes apoptosis induced by ischemia and hypoxia. Conversely, knockdown of lncRNA FAF could promote apoptosis in ischemia-hypoxia cardiomyocytes. Moreover, overexpression of lncRNA FAF could also increase the expression of FGF9. Knockdown of the FGF9 expression could promote apoptosis in cardiomyocytes with the insult of ischemia and hypoxia, which was consistent with the effect of lncRNA FAF overexpression on cardiomyocyte apoptosis. Mechanistically, FGF9 inhibited cardiomyocytes apoptosis through activating signaling tyrosine kinase FGFR2 via phosphoinositide 3-kinase/protein kinase B signaling pathway. Thus, lncRNA FAF plays a protective role in ischemia-hypoxia cardiomyocytes and may serve as a treatment target for AMI. K E Y W O R D S cardiomyocytes apoptosis, FGF9, ischemia-hypoxia, lncRNA FAF Additional supporting information may be found online in the Supporting Information section at the end of the article. How to cite this article: Shi HJ, Wang MW, Sun JT, et al. A novel long noncoding RNA FAF inhibits apoptosis via upregulating FGF9 through PI3K/AKT signaling pathway in ischemia-hypoxia cardiomyocytes.
Porous Pt-M (M = Cu, Zn, Ni) nanoparticles (NPs) were obtained by reduction of [Pt(CH3NH2)4][PtCl4] and M(Ac)2 (or MCl2) with oleylamine under mild conditions. The porous Pt-Cu NPs exhibited superior catalytic activities over a Pt/Cu NP mixture and Cu NPs as references for CO oxidation processes.
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