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A Hollow Microtubular Triazine- and Benzobisoxazole-Based Covalent Organic Framework Presenting Sponge-Like Shells That Functions as a High-Performance Supercapacitor
(2019-05-02)
El-Mahdy, Ahmed F. M.
;
Hung, Ying-Hui
;
Mansoure, Tharwat Hassan
;
Yu, Hsiao-Hua
;
Chen, Tao
In this paper we report the construction of a hollow microtubular triazine- and benzobisoxazole-based covalent organic framework (COF) presenting a sponge-like shell through a template-free [3+2] condensation of the planar molecules 2,4,6-tris(4-formylphenyl)triazine (TPT-3CHO) and 2,5-diaminohydroquinone dihydrochloride (DAHQ-2HCl). The synthesized COF exhibited extremely high crystallinity, a high surface area (ca. 1855m(2)g(-1)), and ultrahigh thermal stability. Interestingly, a time-dependent study of the formation of the hollow microtubular COF having a sponge-like shell revealed a transformation from initial ribbon-like crystallites into a hollow tubular structure, and confirmed that the hollow nature of the synthesized COF was controlled by inside-out Ostwald ripening, while the non-interaction of the crystallites on the outer surface was responsible for the sponge-like surface of the tubules. This COF exhibited significant supercapacitor performance: a high specific capacitance of 256Fg(-1) at a current density of 0.5Ag(-1), excellent cycling stability (98.8% capacitance retention over 1850cycles), and a high energy density of 43Whkg(-1). Such hollow structural COFs with sponge-like shells appear to have great potential for use as high-performance supercapacitors in energy storage applications.
Conducting Ag/oligothiophene complex pastes through a simple quenching/chelation method
(2014-08-14)
Lu, Fang-Hsien
;
Chang, Feng-Chih
;
Mohamed, Mohamed-Gamal
;
Liu, Tzeng-Feng
;
Chao, Chuen-Guang
This paper describes a simple and environmentally friendly approach-a facile, one-pot, quenching/ chelation method-for the fabrication of a silver paste in the form of Ag/oligothiophene complex composites. These Ag/oligothiophene complex composites possess excellent conductivities of 1.8 x 10(4) S cm(-1) in the bulk state and 6.08 x 10(2) S cm(-1) in the form of thin films. We have used X-ray diffraction (XRD). X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and scanning electron microscopy (SEM) to characterize the microstructures of these novel Ag/oligothiophene complex composites.
Improved reliability from a plasma-assisted metal-insulator-metal capacitor comprising a high-k HfO2 film on a flexible polyimide substrate
(2010-01-01)
Meen, Jagan Singh
;
Chu, Min-Ching
;
Kuo, Shiao-Wei
;
Chang, Feng-Chih
;
Ko, Fu-Hsiang
We have used a sol-gel spin-coating process to fabricate a new metal-insulator-metal (MIM) capacitor comprising a 10 nm-thick high-k thin dielectric HfO2 film on a flexible polyimide (PI) substrate. The surface morphology of this HfO2 film was investigated using atomic force microscopy and scanning electron microscopy, which confirmed that continuous and crack-free film growth had occurred on the film surface. After oxygen (O-2) plasma pretreatment and subsequent annealing at 250 degrees C, the film on the PI substrate exhibited a low leakage current density of 3.64 x 10(-9) A cm(-2) at 5 V and a maximum capacitance density of 10.35 fF mu m(-2) at 1 MHz. The as-deposited sol-gel film was completely oxidized when employing O2 plasma at a relatively low temperature (ca. 250 degrees C), thereby enhancing the electrical performance. We employed X-ray photoelectron spectroscopy (XPS) at both high and low resolution to examine the chemical composition of the film subjected to various treatment conditions. The shift of the XPS peaks towards higher binding energy, revealed that O-2 plasma treatment was the most effective process for the complete oxidation of hafnium atoms at low temperature. A study of the insulator properties indicated the excellent bendability of our MIM capacitor; the flexible PI substrate could be bent up to 10(5) times and folded to near 360 degrees without any deterioration in its electrical performance.
Strong Hydrogen Bonding with Inorganic Pendant Polyhedral Oligomeric Silsesquioxane Nanoparticles Provides High Glass Transition Temperature Poly(methyl methacrylate) Copolymers
(2018-01-01)
Yeh, Shu-Ling
;
Zhu, Chao-Yuan
;
Kuo, Shiao-Wei
;
應用化學系
;
Department of Applied Chemistry
We report a series of poly(methyl methacrylate) (PMMA) copolymers containing small amounts of methacrylamide (MAAM) and pendant polyhedral oligomeric silsesquioxane (POSS) methyl acrylate (MAPOSS) segments. The hydrogen bonding interactions of the MAAM monomer units and the inorganic POSS nanoparticle units improved the thermal and mechanical properties of the PMMA copolymers. For example, PMMA copolymerization with 5 wt% PMAAM and 5 wt% PMAPOSS monomers could enhance the glass transition temperature to 142 degrees C, with higher modulus, higher water contact angle, and reasonably high transparency. Such copolymers have potential to replace PMMA homopolymers in optical applications.
Stimuli-responsive supramolecular materials: photo-tunable properties and molecular recognition behavior
(2016)
Huang, Cheng-Wei
;
Wu, Pei-Wei
;
Su, Wei-Hung
;
Zhu, Chao-Yuan
;
Kuo, Shiao-Wei
A new homopolymer of polystyrene (PS) presenting pendant diaminopyridine (DAP) moieties has been prepared using controlled free radical polymerization and a CuAAC "click" reaction. Through directional complementary multiple hydrogen bonding, this PVB-DAP polymer underwent complexation with a thymine-functionalized azobenzene (Azo-T). The resulting supramolecular complex exhibited amorphous and chromophoric behavior without microphase separation. This strategy allowed the fabrication of homogeneous stimuli-responsive thin films with photocontrollable behavior through photoinduced trans-cis isomerization. The PVB-DAP/Azo-T supramolecular complex facilitated the dispersion of an azo-dye through noncovalent interactions; the resulting complex was used to fabricate a surface relief grating displaying an interference pattern. The "recordability" and "rewritability" of these supramolecular complexes suggest that they are promising materials for optical applications and therefore advance the pathway for supramolecular development.
Ternary polybenzoxazine/POSS/SWCNT hybrid nanocomposites stabilized through supramolecular interactions
(2016)
Shih, Hsi-Kang
;
Hsieh, Chun-Cheng
;
Mohamed, Mohamed Gamal
;
Zhu, Chao-Yuan
;
Kuo, Shiao-Wei
In this study we linked zero-dimensional polyhedral oligomeric silsesquioxane (POSS) with one-dimensional single-walled carbon nanotubes (SWCNTs) as dual-dimensional nanohybrid complexes within polybenzoxazine matrices, stabilized through noncovalent supramolecular interactions. First, we synthesized a new bifunctionalized benzoxazine (Py-Bz-T), presenting thymine (T) and pyrene (Py) units, that displayed excellent thermal properties after thermal curing, because its T moieties increased the physical cross-linking density. Second, we prepared Py-Bz-T/OBA-POSS [octuply adenine (A)-functionalized POSS] nanocomposites and investigated, using nuclear magnetic resonance and Fourier transform infrared spectroscopies, the multiple hydrogen bonding A center dot center dot center dot T interactions between Py-Bz-T and OBA-POSS. Finally, we prepared Py-Bz-T/OBA-POSS/SWCNT ternary hybrid complexes dispersed in THF, stabilized through both multiple hydrogen bonding and pi-pi stacking interactions. Transmission electron microscopy revealed that the SWCNTs were highly dispersed and covered by the Py-Bz-T/OBA-POSS nanocomposites; these ternary hybrid complexes were stabilized through pi-pi interactions between Py-Bz-T/OBA-POSS and the SWCNTs, as evidenced using fluorescence spectroscopy.
Functional Supramolecular Polypeptides Involving pi-pi Stacking and Strong Hydrogen-Bonding Interactions: A Conformation Study toward Carbon Nanotubes (CNTs) Dispersion
(2016-08-09)
Huang, Cheng-Wei
;
Mohamed, Mohamed Gamal
;
Zhu, Chao-Yuan
;
Kuo, Shiao-Wei
;
應用化學系
New supramolecular polypeptides have been prepared through simple ring-opening polymerization and "click" reactions. Postfunctionalization with diaminopyridine (DAP) moieties, capable of multiple hydrogen bonding, was an efficient approach toward forming a-helical-dominant polypeptides. The physically cross-linked networks produced upon self-organization of the DAP units increased the glass transition temperature (T-g) of the polymers and sustained the secondary structures of the polypeptides. Additional thermal responsivity resulted from dynamic noncovalent bonding on the polymer side chains. Molecular recognition through heterocomplementary DAP thymine (T) base pairs was revealed spectroscopically and then used to construct poly(y-propargylL-glutamate)-g-N-(6-acetamidopyridin-2-y1)-11-undecanamide/thyminylpyrene (PPLG-DAP/Py-T) supramolecular complexes. Transmission electron microscopy images revealed that this complex was an efficient dispersant of carbon nanotubes (CNTs). Indeed, it could disperse CNTs in both polar and nonpolar media, the direct result of combining two modes of secondary noncovalent bonding: multiple hydrogen bonding and pi-pi interactions. Furthermore, CNT composites fabricated with biocompatible polymers and high value of T-g should enable the development of bio-inspired carbon nanostructures and lead the way toward their biomedical applications.
Supramolecular control over the morphology of bio-inspired poly(3-hexylthiophene) for organic thin film transistors
(2017-02)
Lin, Yen-Ting
;
Singh, Ranjodh
;
Kuo, Shiao-Wei
;
Ko, Fu-Hsiang
;
材料科學與工程學系
We have developed a strategy for modifying the channel layer of organic thin film transistors (OTFTs) through side-chain induced self-organization into a well-ordered film. To obtain selectively self-patterned layers, we treated an adenine-functionalized poly(3-hexylthiophene) (PAT) with adenosine triphosphate (ATP). Using this strategy, interchain charge transport resulting from pi-conjugation was selected to control the polymer morphology, without the need of additional chemical synthetic processing. The side chain-induced self-organization can be understood in terms of supramolecular interactions. The pi-electrons were delocalized among the thiophene rings, thereby improving the interchain charge transport ability; the resulting planar pi-electron system in PAT: ATP resulted in closer intermolecular pep distances, facilitating enhanced charge carrier mobility within a fibrillar structure. The PAT: ATP-based OTFT device exhibited moderate to improved electronic characteristics, with an average field mobility of 3.2 x 10(-4) cm(2) V-1 s(-1) at -30 V and a threshold voltage (V-th) of 5 V, and an on/off current ratio of 10(6). This method has great potential for inducing selective intermolecular interactions in fully solution processed electronic devices. (C) 2016 Elsevier B.V. All rights reserved.
Stimuli-responsive supramolecular materials: photo-tunable properties and molecular recognition behavior
(2016-01-01)
Huang, Cheng-Wei
;
Wu, Pei-Wei
;
Su, Wei-Hung
;
Zhu, Chao-Yuan
;
Kuo, Shiao-Wei
A new homopolymer of polystyrene (PS) presenting pendant diaminopyridine (DAP) moieties has been prepared using controlled free radical polymerization and a CuAAC "click" reaction. Through directional complementary multiple hydrogen bonding, this PVB-DAP polymer underwent complexation with a thymine-functionalized azobenzene (Azo-T). The resulting supramolecular complex exhibited amorphous and chromophoric behavior without microphase separation. This strategy allowed the fabrication of homogeneous stimuli-responsive thin films with photocontrollable behavior through photoinduced trans-cis isomerization. The PVB-DAP/Azo-T supramolecular complex facilitated the dispersion of an azo-dye through noncovalent interactions; the resulting complex was used to fabricate a surface relief grating displaying an interference pattern. The "recordability" and "rewritability" of these supramolecular complexes suggest that they are promising materials for optical applications and therefore advance the pathway for supramolecular development.
A cross-linkable triphenylamine derivative as a hole injection/transporting material in organic light-emitting diodes
(2015-01-01)
Shih, Hsi-Kang
;
Chu, Yu-Lin
;
Chang, Feng-Chih
;
Zhu, Chao-Yuan
;
Kuo, Shiao-Wei
We have synthesized TPABZ, a new thermally cross-linkable triphenylamine derivative containing a benzoxazine functional group, for application in organic light-emitting diodes (OLEDs). We used differential scanning calorimetry, thermogravimetric analysis, UV-Vis spectroscopy, and cyclic voltammetry to investigate the thermal, physical, and electrochemical properties of TPABZ, which is readily polymerized, through ring-opening polymerization of its benzoxazine unit, upon heating at 220 degrees C for 30 min. The cured TPABZ (P-TPABZ) is suitable for use as a hole injection/transport material in OLEDs because it has an appropriate HOMO energy level (-5.16 eV) to form a stepwise energy ladder and a high LUMO energy level (-1.68 eV) with great potential for electron blocking. We fabricated multilayered OLEDs (ITO/TPABZ or P-TPABZ/NPB/Alq(3)/LiF/Al) through successive spin-coating and vacuum deposition processes; the device incorporating P-TPABZ exhibited good performance (EQE: 2.44%; LEmax: 8.42 cd A(-1); PEmax: 4.34 lm W-1).

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