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71.
Arene-fluoroarene interactions offer outstanding possibilities for engineering of supramolecular systems, including nucleic acids. Here, we implement the tolane-perfluorotolane interaction as base pair replacement in DNA. Tolane (THH) and perfluorotolane (TFF) moieties were connected to acyclic backbone units, comprising glycol nucleic acid (GNA) or butyl nucleic acid (BuNA) building blocks, that were incorporated via phosphoramidite chemistry at opposite positions in a DNA duplex. Thermodynamic analyses by UV thermal melting revealed a compelling stabilization by THH/TFF heteropairs only when connected to the BuNA backbone, but not with the shorter GNA linker. Detailed NMR studies confirmed the preference of the BuNA backbone for enhanced polar π-stacking. This work defines how orthogonal supramolecular interactions can be tailored by small constitutional changes in the DNA backbone, and it inspires future studies of arene-fluoroarene-programmed assembly of DNA.  相似文献   
72.
Oxygen evolution reaction (OER) is the most critical step in water splitting, still limiting the development of efficient alkaline water electrolyzers. Here we investigate the OER activity of Au–Fe nanoalloys obtained by laser-ablation synthesis in solution. This method allows a high amount of iron (up to 11 at %) to be incorporated into the gold lattice, which is not possible in Au–Fe alloys synthesized by other routes, due to thermodynamic constraints. The Au0.89Fe0.11 nanoalloys exhibit strongly enhanced OER in comparison to the individual pure metal nanoparticles, lowering the onset of OER and increasing up to 20 times the current density in alkaline aqueous solutions. Such a remarkable electrocatalytic activity is associated to nanoalloying, as demonstrated by comparative examples with physical mixtures of gold and iron nanoparticles. These results open attractive scenarios to the use of kinetically stable nanoalloys for catalysis and energy conversion.  相似文献   
73.
Some new 1,2,3-triazolo[4,5-e]-1,2,4-triazolo[3, 4 -c]pyrimidmes were prepared starting from the corresponding 1,2,3-triazolo[4,5-d]pyrimidines via the formation of the 1,2,4-triazole ring. Thus suitable hydrazino derivatives 6 were condensed with triethyl orthoformate, triethyl orthoacetate and triethyl orthobenzoate to give the expected tricyclic derivatives 7 , 8 and 9 . Intramolecular cyclization of the ethoxycarbonylhydrazino derivatives 10 gave the tricyclic compounds 11 bearing an hydroxyl group in the 3 position. The v-triazolo-s-triazolopyrimidine derivatives were tested towards the A1 and A2A adenosine receptors in binding assays, but they did not show any receptor affinity.  相似文献   
74.
The radical and polymer chain length distributions and their respective convolutes were calculated for any combination of an initiation period followed by a dark period without any initiation. The distributions are characterized by the appearance of an asymmetric (broad) additional peak. The choice of the experimental parameters (i. e. duration of the initiation and the dark period) influences the location of the peak as well as the extension of the complete distribution curve. The first and second derivatives also show a characteristic pattern in the region of the peak. A single experiment yields at least two kp-values which are determined from different parts of the distribution. These values have to be identical unless kp is not characterized by a single value. In principle, a single experiment will suffice to display possible irregularities in kp-constancy.  相似文献   
75.
All-electron ab initio Hartree–Fock (HF ), valence configuration interaction (CI ), and multiconfiguration self-consistent-field (CASSCF ) calculations have been applied to investigate the electronic states of the CrC molecule. The molecule is predicted as having four low-lying electronic states, 3?, 5?, 7?, and 9?, separated by an energy gap of 0.55 eV from the next higher-lying state, 1?, which is followed by the states 5Π and 7Π. The four lowest-lying electronic states are due to the coupling of the angular momenta of the 6Sg Cr+ ion with those of the 4Su C? anion. The chemical bond in the 3? ground state can be viewed as a quadruple bond composed of two σ and two π bonds. One σ bond is due to the formation of a molecular orbital that is doubly occupied. The remaining bonds, i.e., one σ and two π bonds, arise from valence-bond couplings. The π bonds originate from the valence-bond couplings of the electrons in the C 2pπ orbitals with those in the Cr 3dπ orbitals. The σ bond originates from the valence-bond coupling of the C 2pσ electron with an electron in the Cr 4s, 4p hybrid that is polarized away from the C atom.  相似文献   
76.
Annali di Matematica Pura ed Applicata (1923 -) - We obtain convolution inequalities in Lebesgue and Lorentz spaces with power weights when the functions involved are assumed to be radially...  相似文献   
77.
In this paper we study the controllability for a class of semilinear differential inclusions in Banach spaces. Since we assume the regularity of the nonlinear part with respect to the weak topology, we do not require the compactness of the evolution operator generated by the linear part. As well we are not posing any conditions on the multivalued nonlinearity expressed in terms of measures of noncompactness. We are considering the usual assumption on the controllability of the associated linear problem. Notice that, in infinite dimensional spaces, the above mentioned compactness of the evolution operator and linear controllability condition are in contradiction with each other. We suppose that the nonlinear term has convex, closed, bounded values and a weakly sequentially closed graph when restricted to its second argument. This regularity setting allows us to solve controllability problem under various growth conditions. As application, a controllability result for hyperbolic integro-differential equations and inclusions is obtained. In particular, we consider controllability of a system arising in a model of nonlocal spatial population dispersal and a system governed by the second order one-dimensional telegraph equation.  相似文献   
78.
On the Effect of Misspecifying the Density Ratio Model   总被引:1,自引:0,他引:1  
The density ratio model specifies that the log-likelihood ratio of two unknown densities is of known linear form which depends on some finite dimensional parameters. The model can be broadened to allow for m-samples in a quite natural way. Estimation of both parametric and nonparametric part of the model is carried out by the method of empirical likelihood. However the assumed linear form has an impact on the estimation and testing for the parametric part. The goal of this study is to quantify the effect of choosing an incorrect linear form and its impact to inference. The issue of misspecification is addressed by embedding the unknown linear form to some parametric transformation family which yields ultimately to its identification. Simulated examples and data analysis integrate the presentation.  相似文献   
79.
LetM be a compact orientable surface,I:M R4 an immersion of classC r and a normal unitary smooth vector field. We prove that in the space of pairs (I, ) the family of pairs all whose umbilical points are Darbouxian is generic.  相似文献   
80.
We discuss a major change in the way we teach our first-year statistics course. We have redesigned this course with emphasis on teaching critical thinking. We recognized that most of the students take the course for general knowledge and support of other majors, and very few are planning to major in statistics. We identified the essential aspects of a first-year statistics course, given this student mix, focusing on a simple question, ‘Given this is the last chance you have to teach statistics, what are the essential skills students need?’ We have moved from thinking about statistics skills needed for a statistician to skills needed to participate in today's society. We have changed the way we deliver the course with less emphasis on lectures and more on alternative resources including on-line tutorials, Excel, computer-based skills testing, web-based learning materials and smaller group activities such as study groups and example classes. Feedback from students shows that they are very receptive and enthusiastic.  相似文献   
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