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1.
Solvent Influence on Cellulose 1,4‐β‐Glycosidic Bond Cleavage: A Molecular Dynamics and Metadynamics Study 下载免费PDF全文
Claudia Loerbroks Eliot Boulanger Prof. Dr. Walter Thiel 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(14):5477-5487
We explore the influence of two solvents, namely water and the ionic liquid 1‐ethyl‐3‐methylimidazolium acetate (EmimAc), on the conformations of two cellulose models (cellobiose and a chain of 40 glucose units) and the solvent impact on glycosidic bond cleavage by acid hydrolysis by using molecular dynamics and metadynamics simulations. We investigate the rotation around the glycosidic bond and ring puckering, as well as the anomeric effect and hydrogen bonds, in order to gauge the effect on the hydrolysis mechanism. We find that EmimAc eases hydrolysis through stronger solvent–cellulose interactions, which break structural and electronic barriers to hydrolysis. Our results indicate that hydrolysis in cellulose chains should start from the ends and not in the centre of the chain, which is less accessible to solvent. 相似文献
2.
We develop a mechanical theory for systems of rod-like particles. Central to our approach is the assumption that the external power expenditure for any subsystem of rods is independent of the underlying frame of reference. This assumption is used to derive the basic balance laws for forces and torques. By considering inertial forces on par with other forces, these laws hold relative to any frame of reference, inertial or noninertial. Finally, we introduce a simple set of constitutive relations to govern the interactions between rods and find restrictions necessary and sufficient for these laws to be consistent with thermodynamics. Our framework provides a foundation for a statistical mechanical derivation of the macroscopic balance laws governing liquid crystals. 相似文献
3.
Working on a state space determined by considering a discrete system of rigid rods, we use nonequilibrium statistical mechanics to derive macroscopic balance laws for liquid crystals. A probability function that satisfies the Liouville equation serves as the starting point for deriving each macroscopic balance. The terms appearing in the derived balances are interpreted as expected values and explicit formulas for these terms are obtained. Among the list of derived balances appear two, the tensor moment of inertia balance and the mesofluctuation balance, that are not standard in previously proposed macroscopic theories for liquid crystals but which have precedents in other theories for structured media. 相似文献
4.
Hans Eliot Edling Matthew Vincent Herv Marand Samantha J. Talley Kevin Barr Robert B. Moore S. Richard Turner 《Journal of Polymer Science.Polymer Physics》2019,57(15):973-980
Structurally rigid copolyester thermoplastics were synthesized from 1,4‐cyclohexanedimethanol and the diesters dimethyl biphenyl‐4,4′‐dicarboxylate and dimethyl 2,6‐naphthalenedicarboxylate (DMN) via conventional melt transesterification. Conventional differential scanning calorimetry (CDSC) showed all compositions to exhibit multiple endotherms upon heating. Wide‐angle X‐ray diffraction analysis showed copolyester compositions to exhibit the crystalline structure of either the homopolyester Poly(1,4‐cyclohexylenedimethylene 2,6‐naphthalate) (PCN) or the homopolyester Poly(1,4‐cyclohexylenedimethylene 4,4′‐bibenzoate) (PCB), but not both simultaneously. Further thermal analysis using CDSC and fast DSC investigated the origin of the multiple endotherm behavior. While three endotherms are observed for low heating rates, the upper two endotherms appear to merge at heating rates about 1–5 °C s?1 and a single endotherm remains above heating rates about 10–50 °C s?1. While the behavior of the upper two endotherms is undeniably consistent with the mechanism of melting–recrystallization–remelting (MRR), we suggest that the low endotherm is likely associated with the melting of constrained secondary crystals, although MRR effects cannot be ruled out. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57, 973–980 相似文献
5.
Mia Kurek Nasreddine Benbettaieb Mario
etar Eliot Chaudy Maja Repaji Damir Klepac Sreko Vali Frdric Debeaufort Kata Gali 《Molecules (Basel, Switzerland)》2021,26(9)
Chitosan and pectin films were enriched with blackcurrant pomace powder (10 and 20% (w/w)), as bio-based material, to minimize food production losses and to increase the functional properties of produced films aimed at food coatings and wrappers. Water vapor permeability of active films increased up to 25%, moisture content for 27% in pectin-based ones, but water solubility was not significantly modified. Mechanical properties (tensile strength, elongation at break and Young’s modulus) were mainly decreased due to the residual insoluble particles present in blackcurrant waste. FTIR analysis showed no significant changes between the film samples. The degradation temperatures, determined by DSC, were reduced by 18 °C for chitosan-based samples and of 32 °C lower for the pectin-based samples with blackcurrant powder, indicating a disturbance in polymer stability. The antioxidant activity of active films was increased up to 30-fold. Lightness and redness of dry films significantly changed depending on the polymer type. Significant color changes, especially in chitosan film formulations, were observed after exposure to different pH buffers. This effect is further explored in formulations that were used as color change indicators for intelligent biopackaging. 相似文献
6.
The remarkable ability of nematic elastomers to exhibit large deformations under small applied forces is known as soft elasticity.
The recently proposed neo-classical free-energy density for nematic elastomers, derived by molecular-statistical arguments,
has been used to model soft elasticity. In particular, the neo-classical free-energy density allows for a continuous spectrum
of equilibria, which implies that deformations may occur in the complete absence of force and energy cost. Here we study the
notion of force-free states in the context of a continuum theory of nematic elastomers that allows for isotropy, uniaxiality,
and biaxiality of the polymer microstructure. Within that theory, the neo-classical free-energy density is an example of a
free-energy density function that depends on the deformation gradient only through a nonlinear strain measure associated with
the deformation of the polymer microstructure relative to the macroscopic continuum. Among the force-free states for a nematic
elastomer described by the neo-classical free energy density, there is, in particular, a continuous spectrum of states parameterized
by a pair of tensors that allows for soft deformations. In these force-free states the polymer microstructure is material
in the sense that it stretches and rotates with the macroscopic continuum. Limitations of and possible improvements upon the
neo-classical model are also discussed.
This revised version was published online in July 2006 with corrections to the Cover Date. 相似文献
7.
Shi W Petersen EB Nguyen DT Yao Z Chavez-Pirson A Peyghambarian N Yu J 《Optics letters》2011,36(18):3575-3577
We report a unique all fiber-based single-frequency Q-switched laser in a monolithic master oscillator power amplifier configuration at ~1920 nm by using highly Tm-doped germanate fibers for the first time. The actively Q-switched fiber laser seed was achieved by using a piezo to press the fiber in the fiber Bragg grating cavity and modulate the fiber birefringence, enabling Q-switching with pulse width and repetition rate tunability. A single-mode polarization maintaining large core 25 μm highly Tm-doped germanate fiber was used in the power amplifier stage. For 80 ns pulses with 20 kHz repetition rate, we achieved 220 μJ pulse energy, which corresponds to a peak power of 2.75 kW with transform-limited linewidth. 相似文献
8.
We formulate integral statements of force balance, energy balance, and entropy imbalance for an interface between a body and
its environment. These statements account for interfacial energy, entropy, and stress but neglect the inertia of the interface.
Our final results consist of boundary conditions describing thermomechanical interactions between the body and its environment.
In their most general forms, these results are partial differential equations that account for dissipation and encompass as
special cases Navier’s slip law, Newton’s law of cooling, and Kirchhoff’s law of radiation. When dissipation is neglected,
our results reduce to the well-known zero-slip, free-surface, zero-shear, prescribed temperature, and flux-free conditions.
Dedicated to James K. Knowles: teacher, colleague, friend 相似文献
9.
10.
The Galois group of the splitting field of an irreducible binomialx
2e
−a overQ is computed explicitly as a full subgroup of the holomorph of the cyclic group of order 2
e
. The general casex
n
−a is also effectively computed. 相似文献