We demonstrate in this article the facile synthesis of a novel range of "treelike" polyethylene block polymers constructed uniquely with chain blocks of hybrid hyperbranched-linear chain topologies from sole ethylene stock. Though chemically identical, the blocks in the polymers are featured with distinctly different chain topologies, varying from hyperbranched to linear. This synthesis is achieved uniquely through one-pot stagewise chain walking ethylene "living" polymerization with a Pd-diimine catalyst, [(ArNd, under varying conditions. It takes advantage of the combined outstanding features of the Pd-diimine catalyst in ethylene polymerization; the "living" polymerization behavior at a broad range of ethylene pressure and temperature and the capability of topology tuning by changing both parameters. In this stagewise "living" polymerization technique, the polymerization condition (ethylene pressure and temperature) is varied from stage to stage to grow blocks of different desired topologies while with maintained "living" behavior. With this technique, diblock polymers, containing a hyperbranched first block and a linear second block with controllable narrowdistributed sizes, have been obtained through two-stage polymerizations using the growth order of "hyperbranched-first" with the first stage at 1 atm/15 °C and the second stage at 27 atm/5 °C. The distinct block structure in these diblock polymers is verified based on the fact that their intrinsic viscosity data follow consistently the combination rule found with conventional diblock polymers. In addition, the synthesis of triblock polymers, composed of a hyperbranched first block, a medium-compact second block, and a linear third block, is also demonstrated through three-stage polymerization involving the first stage at 1 atm/15 °C, the second at 3 atm/15 °C, and the third at 27 atm/5 °C.
In this work, few layer graphene quantum dots (GQDs) with a size of 3-5 nm are purposely treated with highly concentrated aqueous NaBH4 solutions to obtain the reduced graphene quantum dots (rGQDs). Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy demonstrate that the number of carbonyl groups decreases but -OH related defects increase during chemical reduction. Green and weak emissions of original GQDs originate from carrier recombination in the disorder-induced localized state (mainly including carbonyl and carboxyl and epoxy groups). As the reduction degree increases, the photoluminescence (PL) quantum efficiency of GQDs increases dramatically from 2.6% to 10.1%. In the meantime, the PL peak position blue shifts rapidly, and full width at half maximum (FWHM) becomes narrower. Thus we can infer that graphenol topological defects (hydroxyl functionalized graphene) are gradually formed during reduction. Besides, graphenol defect related PL features a longer fluorescence lifetime, excitation wavelength dependence but less pH sensitivity.
A two-dimensional red blood cell (RBC) membrane model based on elastic and Euler–Bernoulli beam theories is introduced in the frame of immersed boundary-lattice Boltzmann method (IB-LBM). The effect of the flexible membrane is handled by the immersed boundary method in which the stress exerted by the RBC on the ambient fluid is spread onto the collocated grid points near the boundary. The fluid dynamics is obtained by solving the discrete lattice Boltzmann equation. A "ghost shape", to which the RBC returns when restoring, is introduced by prescribing a bending force along the boundary. Numerical examples involving tumbling, tank-treading and RBC aggregation in shear flow and deformation and restoration in poiseuille flow are presented to verify the method and illustrate its efficiency. As an application of the present method, a ten-RBC colony being compressed through a stenotic microvessel is studied focusing the cell–cell interaction strength. Quantitative comparisons of the pressure and velocity on specified microvessel interfaces are made between each aggregation case. It reveals that the stronger aggregation may lead to more resistance against blood flow and result in higher pressure difference at the stenosis.
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