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The structure and rotational barrier for the mesityl-silicon bond of 2,2-dimesityl-1,1,1,3,3,3-hexamethyltrisilane have been investigated by 1H- and 13C-variable temperature nuclear magnetic resonance (NMR) as well as by density functional theory structural calculations. The calculations show that the lowest energy structure has C2 symmetry with nonequivalent ortho methyl groups, consistent with the crystal structure and solution NMR. The nonequivalent ortho methyl groups exchange through a Cs transition state with a calculated relative free energy of 11.0 kcal mol−1. The barrier for this rotation found by dynamic NMR is 13.4 ± 0.2 kcal mol−1 at 298 K. 相似文献
3.
Yeong‐Tarng Shieh Pei‐Yu Tai Chih‐Chia Cheng 《Journal of polymer science. Part A, Polymer chemistry》2019,57(21):2149-2156
Poly(methyl methacrylate) (PMMA) nanoparticles with a sensitive CO2‐responsive hydrophilic/hydrophobic surface that confers controlled dispersion and aggregation in water were prepared by emulsion polymerization at 50 °C under CO2 bubbling using amphiphilic diblock copolymers of 2‐dimethylaminoethyl methacrylate (DMAEMA) and N‐isopropyl acrylamide (NIPAAm) as an emulsifier. The amphiphilicity of the hydrophobic–hydrophilic diblock copolymer at 50 °C was triggered by CO2 bubbling in water and enabled the copolymer to serve as an emulsifier. The resulting PMMA nanoparticles were spherical, approximately 100 nm in diameter and exhibited sensitive CO2/N2‐responsive dispersion/aggregation in water. Using copolymers with a longer PNIPAAm block length as an emulsifier resulted in smaller particles. A higher concentration of copolymer emulsifier led to particles with a stickier surface. Given its simple preparation and reversible CO2‐triggered amphiphilic behavior, this newly developed block copolymer emulsifier offers a highly efficient route toward the fabrication of sensitive CO2‐stimuli responsive polymeric nanoparticle dispersions. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 2149–2156 相似文献
4.
Dr. Liat Avram Dr. Václav Havel Ronit Shusterman-Krush Dr. Mark A. Iron Dr. Moritz Zaiss Prof. Vladimír Šindelář Dr. Amnon Bar-Shir 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(7):1687-1690
The accumulated knowledge regarding molecular architectures is based on established, reliable, and accessible analytical tools that provide robust structural and functional information on assemblies. However, both the dynamicity and low population of noncovalently interacting moieties within studied molecular systems limit the efficiency and accuracy of traditional methods. Herein, the use of a saturation transfer-based NMR approach to study the dynamic binding characteristics of an anion to a series of synthetic receptors derived from bambusuril macrocycles is demonstrated. The exchange rates of BF4− are mediated by the side chains on the receptor (100 s−1<kex<5000 s−1), which play a critical role in receptor-anion binding dynamics. The signal amplification obtained with this approach allows for the identification of different types of intermolecular interactions between the receptor and the anion, something that could not have been detected by techniques hitherto used to study molecular assemblies. These findings, which are supported by a computational molecular dynamic study, demonstrate the uniqueness and added value of this NMR method. 相似文献
5.
Markus Bödenler Ludovic de Rochefort P. James Ross Nicolas Chanet Geneviève Guillot Gareth R. Davies 《Molecular physics》2019,117(7-8):832-848
ABSTRACTFast field-cycling (FFC) nuclear magnetic resonance relaxometry is a well-established method to determine the relaxation rates as a function of magnetic field strength. This so-called nuclear magnetic relaxation dispersion gives insight into the underlying molecular dynamics of a wide range of complex systems and has gained interest especially in the characterisation of biological tissues and diseases. The combination of FFC techniques with magnetic resonance imaging (MRI) offers a high potential for new types of image contrast more specific to pathological molecular dynamics. This article reviews the progress in FFC-MRI over the last decade and gives an overview of the hardware systems currently in operation. We discuss limitations and error correction strategies specific to FFC-MRI such as field stability and homogeneity, signal-to-noise ratio, eddy currents and acquisition time. We also report potential applications with impact in biology and medicine. Finally, we discuss the challenges and future applications in transferring the underlying molecular dynamics into novel types of image contrast by exploiting the dispersive properties of biological tissue or MRI contrast agents. 相似文献
6.
In this paper, we consider a viscoelastic wave equation of variable coefficients in the presence of past history with nonlinear damping and delay in the internal feedback and dynamic boundary conditions. Under suitable assumptions, we establish an explicit and general decay rate result without imposing restrictive assumption on the behavior of the relaxation function at infinity by Riemannian geometry method and Lyapunov functional method. 相似文献
7.
电路过渡过程所列方程是微分方程,本文中采用的是方框图模型分析法,即将微分方程的复杂示解分解成最基本的加(减)、乘(除)、积分(微分)、增益等运算,采用VB设计用户界面产进行计算,并给出了一算例。 相似文献
8.
We consider a resource management problem in which the management objective is to minimize fluctuations in resource stocks. Stabilizing management policies constitute the designing of memoryless state feedback control strategies for a discrete time resource model which contains unknown but bounded fluctuations. We also show that the problem of maximizing sustainable yield in an uncertain fishery can be considered as the problem of stabilizing of the stock level.The paper corresponds to an invited talk at the 14th Symposium on Operations Research, Ulm, September 6–8, 1989.The support by Yrjö Jahnsson Foundation is gratefully acknowledged.This work was supported by NSF and AFOSR under grant ECS 8602524. 相似文献
9.
10.
Papert's (1978) appeal to reconsider the power and possibilities of the aesthetic in mathematics learning is often ignored in mathematics education research. This paper begins with the premise, put forth by Dewey (1934), that the aesthetic structures many dimensions of inquiry and experience. In the same way that using particular paintings, musical compositions, or even everyday experiences has been instrumental to attempts by philosophers to understand the aesthetic dimensions of meaning and experience in artistic domains, I propose that analysing a particular encounter with mathematics may help reveal the nature and role of the often nebulous responses of elegance, beauty, and `fit' to which mathematicians lay claim in their mathematical activity. To achieve this, I draw on and adapt the defining features of the aesthetic character of experience set forth by the aesthetician Beardsley (1982). This, in turn, sheds light on the role thataesthetics can play in mathematical inquiry and experience, and provides initial categories and conjectures that can be used to investigate the potential roles of aesthetics in mathematics learning contexts.This revised version was published online in September 2005 with corrections to the Cover Date. 相似文献