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Self-assembly of an A-B diblock copolymer blended with a C homopolymer and a C-D diblock copolymer through hydrogen bonding interaction
(2010-08-19)
Chen, Wan-Chun
;
Kuo, Shiao-Wei
;
Chang, Feng-Chih
;
應用化學系
;
Department of Applied Chemistry
In this study, we investigated the miscibility, phase behavior, and self-assembled nanostructures formed from the immiscible crystalline-amorphous diblock copolymer poly(epsilon-caprolactone-b-4-vinyl pyridine) (PCL-b-P4VP, A-B) when blended with the homopolymer poly(vinyl phenol) (PVPh, C) and the diblock copolymer poly(vinyl phenol-b-styrene) (PVPh-b-PS, C-D). Long-range-ordered microphase separation was difficult to achieve in the PCL-b-P4VP/PVPh (A-B/C) blend system because PVPh interacted with both the P4VP and PCL blocks simultaneously through hydrogen bonding interactions. In contrast, we observed sharp, multiple orders of diffraction in the SAXS profiles of the PCL-b-P4VP/PVPh-b-PS (A-B/C D) blend system, indicating that perfect microphase separation occurred because the incorporation of the PS block induced the PVPh block to hydrogen bond preferentially with the P4VP block. This simple A-B/C-D (PCL-b-P4VP/PVPh-b-PS) diblock copolymer mixture exhibited self-assembly behavior (a three-lamella phase) similar to that of a corresponding ABC triblock copolymer. (C) 2010 Elsevier Ltd. All rights reserved.
Substituent-induced delocalization effects on hydrogen-bonding interaction in poly(N-phenyl methacrylamide) derivatives
(2011-05-26)
Kuo, Shiao-Wei
;
Lin, Chien-Ting
;
Chen, Jem-Kun
;
Ko, Fu-Hsiang
;
Chang, Feng-Chih
Within small molecules, the hydrogen-bonding behaviors affected by delocalization have been studied thoroughly, but rare publication in macromolecules. Therefore, three poly(N-phenyl methacrylamide)s, poly(N-phenyl methacrylamide) (PNPAA), poly(N-4-methoxyphenyl methacrylamide) (PMPMA) and poly(N-4-bromophenyl methacrylamide) (PBPMA), with different inductive substitution at para position of benzene ring are prepared to investigate the substituent-induced delocalization effects on the hydrogen-bonding interaction behaviors. In this study, the variable-temperature FTIR spectrum is used as tool to study the self- and inter-association hydrogen-bonding interaction. FTIR analyses could provide evidences that there is relatively stronger inter-associative hydrogen bonding in poly(N-4-bromophenyl methacrylamide)/P4VP blends. High resolution (13)C CP/MAS solid-state NMR analyses indicate that the spin-lattice relaxation time (T) in all PBPMA blends are homogeneous on the scale at which spin-diffusion occurs within the time T(1)rho(H), also due to the enhancement by substituent inductive delocalization. (C) 2011 Elsevier Ltd. All rights reserved.
Hydrogen bond mediated supramolecular micellization of diblock copolymer mixture in common solvents
(2009-07-01)
Kuo, Shiao-Wei
;
Tung, Pao-Hsaing
;
Chang, Feng-Chih
;
應用化學系
;
Department of Applied Chemistry
We report a new approach toward preparing self-assembled hydrogen-bonded complexes having vesicle and patched spherical structures from two species of block copolymers in nonselective solvents. Two diblock copolymers, poly(styrene-b-vinyl phenol) (PS-b-PvPh) and poly(methyl methacrylate-b-4-vinylpyridine) (PMMA-b-P4VP), were synthesized through anionic polymerization. The assembly of vesicles from the intermolecular complex formed after mixing PS-b-PVPH with PMMA-b-P4VP in THF was driven by strong hydrogen bonding between the complementary binding sites on the PVPH and P4VP blocks. In contrast, well-defined patched spherical micelles formed after blending PS-b-PVPh with PMMA-b-P4VP in DMF: the weaker hydrogen bonds formed between the PVPh and P4VP blocks in DMF, relative to those in THF, resulted in the formation of spherical micelles having compartmentalized coronas consisting of PS and PMMA blocks. (C) 2009 Elsevier Ltd. All rights reserved.
Self-Assembly structures through competitive interactions of miscible crystalline-amorphous diblock copolymer/homopolymer blends
(2009-10-20)
Lin, I-Hong
;
Kuo, Shiao-Wei
;
Chang, Feng-Chih
;
應用化學系
;
Department of Applied Chemistry
A series of miscible crystalline-amorphous diblock copolymers, (poly(epsilon-caprolactone)-b-(vinyl phenol), PCL-b-PVPh) were prepared through sequential ring-opening and controlled living free radical (nitroxide-mediated) polymerizations and then blended with poly(vinyl pyrrolidone) (PVP) homopolymer. Specific interactions, miscibility, and self-assembly morphologies mediated by hydrogen bonding interactions of this new A-B/C type blend, were investigated in detail. Micro-phase separation of these miscible PCL-b-PVPh diblock copolymers occurs by blending with PVP through competitive hydrogen bonding interaction in this A-B/C blend. FTIR, XRD, and DSC analyses provide positive evidences that the carbonyl group of PVP is a significantly stronger hydrogen bond acceptor than PCL, thus the PCL block is excluded from the PVPh/PVP miscible phase to form self-assembly structure. (13)C CP/MAS solid-state NMR spectra provide additional evidence confirming that micro-phase separation occurs in the blend system because of the presence of more than two T(1p)(H) values for this A-B/C blend system. According to the result of the FTIR and SAXS results, the smaller molecular weight system contains a greater fraction of the hydrogen-bonded carbonyl group, cause indirectly the high degree of phase separation among these blends. In addition, the SAXS profiles possess a sharp primary peak and highly long range ordered reflections q/q* ratios of 1:2:3 at lower PVP content, an indication of the lamellar structure in the blend which is consistent with TEM image. The phase behavior and morphology shifts from lamellar to cylinder structure with further increase in the PVP content. (C) 2009 Elsevier Ltd. All rights reserved.
Glass transition temperature enhancement of PMMA through copolymerization with PMAAM and PTCM mediated by hydrogen bonding
(2010-02-15)
Lin, Chien-Ting
;
Kuo, Shiao-Wei
;
Huang, Chih-Feng
;
Chang, Feng-Chih
;
應用化學系
A series of poly(methyl methacrylate-co-methacrylamide-co-tricyclodecyl methacrylate) (PMMA-co-PMAAM-co-PTCM) copolymers possessing high glass transition temperatures and high transparency are prepared. By incorporating the aliphatic tricyclodecyl methacrylate moiety into the PMMA-co-PMAA main chain results in high glass transition temperature and high transparency of PMMA-based polymeric material. The TCM content affects the fraction of hydrogen bonding in these terpolymers, small content of TCM does not sacrifice the fraction of hydrogen-bonded association in and does not cause T(g) decrease. The extent of free amide group plays the major role in dictating moisture absorption of terpolymers. The incorporation of TCM significantly reduces the moisture absorption of terpolymers due to its hydrophobic and bulky tricyclodecyl group. In addition, the TCM plays the role of inert diluent to convert portion of the strong self-associated hydrogen bonded amide groups into inter-associated hydrogen bonding between carbonyl groups of ester units and MAAM. (C) 2010 Elsevier Ltd. All rights reserved.

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