Covalent organic frameworks (COFs) are crystalline porous solids with well-defined two- or three-dimensional molecular structures. Although the structural regularity provides this new type of porous material with high potentials in catalysis, no example has been presented so far. Herein, we report the first application of a new COF material, COF-LZU1, for highly efficient catalysis. The easily prepared imine-linked COF-LZU1 possesses a two-dimensional eclipsed layered-sheet structure, making its incorporation with metal ions feasible. Via a simple post-treatment, a Pd(II)-containing COF, Pd/COF-LZU1, was accordingly synthesized, which showed excellent catalytic activity in catalyzing the Suzuki-Miyaura coupling reaction. The superior utility of Pd/COF-LZU1 in catalysis was elucidated by the broad scope of the reactants and the excellent yields (96-98%) of the reaction products, together with the high stability and easy recyclability of the catalyst. We expect that our approach will further boost research on designing and employing functional COF materials for catalysis.
The periodic layers and ordered nanochannels of covalent organic frameworks (COFs) make these materials viable open catalytic nanoreactors, but their low stability has precluded their practical implementation. Here we report the synthesis of a crystalline porous COF that is stable against water, strong acids and strong bases, and we demonstrate its utility as a material platform for structural design and functional development. We endowed a crystalline and porous imine-based COF with stability by incorporating methoxy groups into its pore walls to reinforce interlayer interactions. We subsequently converted the resulting achiral material into two distinct chiral organocatalysts, with the high crystallinity and porosity retained, by appending chiral centres and catalytically active sites on its channel walls. The COFs thus prepared combine catalytic activity, enantioselectivity and recyclability, which are attractive in heterogeneous organocatalysis, and were shown to promote asymmetric C-C bond formation in water under ambient conditions.
Purpose:To evaluate the value of diffusion-weighted imaging (DWI) in distinguishing between benign and malignant breast lesions. Materials and Methods:Fifty-two female subjects (mean age ϭ 58 years, age range ϭ 25-75 years) with histopathologically proven breast lesions underwent DWI of the breasts with a single-shot echo-planar imaging (EPI) sequence using large b values. The computed mean apparent diffusion coefficients (ADCs) of the breast lesions and cell density were then correlated. Results:The ADCs varied substantially between benign breast lesions ((1.57 Ϯ 0.23) ϫ 10 -3 mm 2 /second) and malignant breast lesions ((0.97 Ϯ 0.20) ϫ 10 -3 mm 2 /second). In addition, the mean ADCs of the breast lesions correlated well with tumor cellularity (P Ͻ 0.01, r ϭ -0.542). Conclusion:The ADC would be an effective parameter in distinguishing between malignant and benign breast lesions. Further, tumor cellularity has a significant influence on the ADCs obtained in both benign and malignant breast tumors.
Covalent organic frameworks are a class of crystalline organic porous materials that can utilize π–π-stacking interactions as a driving force for the crystallization of polygonal sheets to form layered frameworks and ordered pores. However, typical examples are chemically unstable and lack intrasheet π-conjugation, thereby significantly limiting their applications. Here we report a chemically stable, electronically conjugated organic framework with topologically designed wire frameworks and open nanochannels, in which the π conjugation-spans the two-dimensional sheets. Our framework permits inborn periodic ordering of conjugated chains in all three dimensions and exhibits a striking combination of properties: chemical stability, extended π-delocalization, ability to host guest molecules and hole mobility. We show that the π-conjugated organic framework is useful for high on-off ratio photoswitches and photovoltaic cells. Therefore, this strategy may constitute a step towards realizing ordered semiconducting porous materials for innovations based on two-dimensionally extended π systems.
Condensation of hydrazine with 1,3,6,8-tetrakis(4-formylphenyl)pyrene under solvothermal conditions yields highly crystalline two-dimensional covalent organic frameworks. The pyrene units occupy the vertices and the diazabutadiene (-C═N-N═C-) linkers locate the edges of rohmbic-shaped polygon sheets, which further stack in an AA-stacking mode to constitute periodically ordered pyrene columns and one-dimensional microporous channels. The azine-linked frameworks feature permanent porosity with high surface area and exhibit outstanding chemical stability. By virtue of the pyrene columnar ordering, the azine-linked frameworks are highly luminescent, whereas the azine units serve as open docking sites for hydrogen-bonding interactions. These synergestic functions of the vertices and edge units endow the azine-linked pyrene frameworks with extremely high sensitivity and selectivity in chemosensing, for example, the selective detection of 2,4,6-trinitrophenol explosive. We anticipate that the extension of the present azine-linked strategy would not only increase the structural diversity but also expand the scope of functions based on this highly stable class of covalent organic frameworks.
Bulk heterojunction solar cells have attracted considerable attention over the past several years due to their potential for low-cost photovoltaic technology. The possibility of manufacturing modules via a standard printing/coating method in a roll-to-roll process in combination with the use of low-cost materials will lead to a watt-peak price of less than 1 US$ within the next few years. [1] Despite the low-cost potential, the power conversion efficiency of bulk heterojunction devices is low compared to inorganic solar cells. Efficiencies in the range of 5-6% have been certified at NREL and AIST usually on devices with small active areas.[2]The current understanding of bulk heterojunction solar cells suggests that the maximum efficiency is in the range of 10-12%.[3] Several reasons for the power conversion efficiency limitation have been identified.[1] Some of the prerequisites for achieving highest efficiencies are donor and acceptor materials with optimized energy levels [highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO)], efficient charge transport in the donor-acceptor blend, efficient charge generation and limited recombination losses. Power conversion efficiency is strongly dependent on charge transport and charge generation, which are dominated by the phase behavior of the donor and acceptor molecules. The resulting, and often unfavorable, nanomorphology of this two-component blend limits the power conversion efficiency of bulk heterojunction solar cells. Precise control of the nanomorphology is very difficult and has been achieved only for a few systems. [4][5][6] The relation between the chemical structure of donor and acceptor materials and the nanomorphology that they form when they are blended is currently not well understood, and as will be shown in this paper, minor changes in the chemical structure can cause major changes in the performance of the materials in organic solar cells.
Recent evidence that the cerebellum is involved in perception and cognition challenges the prevailing view that its primary function is fine motor control. A new alternative hypothesis is that the lateral cerebellum is not activated by the control of movement per se, but is strongly engaged during the acquisition and discrimination of sensory information. Magnetic resonance imaging of the lateral cerebellar output (dentate) nucleus during passive and active sensory tasks confirmed this hypothesis. These findings suggest that the lateral cerebellum may be active during motor, perceptual, and cognitive performances specifically because of the requirement to process sensory data.
People commonly anthropomorphize nonhuman agents, imbuing everything from computers to pets to gods with humanlike capacities and mental experiences. Although widely observed, the determinants of anthropomorphism are poorly understood and rarely investigated. We propose that people anthropomorphize, in part, to satisfy effectance motivation-the basic and chronic motivation to attain mastery of one's environment. Five studies demonstrated that increasing effectance motivation by manipulating the perceived unpredictability of a nonhuman agent or by increasing the incentives for mastery increases anthropomorphism. Neuroimaging data demonstrated that the neural correlates of this process are similar to those engaged when mentalizing other humans. A final study demonstrated that anthropomorphizing a stimulus makes it appear more predictable and understandable, suggesting that anthropomorphism satisfies effectance motivation. Anthropomorphizing nonhuman agents seems to satisfy the basic motivation to make sense of an otherwise uncertain environment.
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