Co-reporter:Yongming Li, Xiuyuan Ni
Electrochimica Acta 2017 Volume 227(Volume 227) pp:
Publication Date(Web):10 February 2017
DOI:10.1016/j.electacta.2017.01.018
•A new supercapacitive material by integrating conjugated polymers with the composite of graphene oxide and Mn3O4 has been synthesized.•The photopolymerization method establishes the interaction in the ternary composite materials.•The conjugated polymers in the doped GPM composite are efficiently doped by HCl solution, thus improving the conductivity of hybrid materials.•The as-prepared material shows the enhanced supercapacitive properties with high specific capacitance and long-term charge-discharge cycling stability.We synthesize a new supercapacitive material by integrating conjugated polymers with the composite of graphene oxide (GO) and Mn3O4 through photopolymerization. The GO-conjugated polymer composite is prepared via in situ photopolymerization of Pyrrole and 3,4-ethylenedioxythiophene on the surface of GO, followed by the hydrothermal synthesis of Mn3O4 to obtain GO-Polymer-Mn3O4 (GPM). In order to optimize the supercapacitive performance of GPM, the GO-conjugated polymer composite is doped by HCl solution to improve the conductivity of the doped GPM composite. The structures of the composites are characterized using transmission electron microscopy, selected-area electron diffraction, field-emission scanning electron microscopy, fourier transform infrared spectroscopy, X-ray diffractometry, thermogravimetric analysis, X-ray photoelectron spectroscopy and Brunauer-Emmett-Teller. The supercapacitive properties of the doped GPM composite are investigated using different electrochemical techniques including cyclic voltammetry, galvanostatic charge-discharge and electrochemical impedance spectroscopy. The doped GPM electrode shows a high specific capacitance and long-term charge-discharge cycling stability.Download high-res image (275KB)Download full-size image
Co-reporter:Wanfeng Liao
Photochemical & Photobiological Sciences (2002-Present) 2017 vol. 16(Issue 8) pp:1211-1219
Publication Date(Web):2017/08/09
DOI:10.1039/C7PP00013H
Photopolymerization, which is one of the most attractive polymerization methods, has been recently studied for the development of new photoinitiators. Herein, we use a binary mixture of titanium dioxide (TiO2) nanoparticles and carboxylic diacid as a novel photoinitiator to initiate the free radical polymerization of vinyl acetate (VAc). The polymerization of VAc is achieved both in aqueous medium and bulk. The initiation mechanism of TiO2/diacids is studied via nuclear magnetic resonance (NMR) spectroscopy using 13C labeled diacids as probing molecules. Further, a universal reaction mechanism is established, where the polymerization of VAc is initiated by the HOOC-R˙ radical, which is generated from the photocatalytic decarboxylation of the diacid. The polymerization kinetics results indicate that the polymerization rate is strongly dependant on the diacid structure. Compared to the use of diacids with an odd number of carbons, it is found that using diacids with an even number of carbons results in the polymerization rate reaching the maximum value faster.
Co-reporter:Penglei Yang;Xun Ma
Journal of Materials Science: Materials in Electronics 2017 Volume 28( Issue 4) pp:3695-3702
Publication Date(Web):31 October 2016
DOI:10.1007/s10854-016-5975-2
We have synthesized poly(N-vinylcarbazole) (PVK) by using graphene oxide (GO) as photo-initiator and obtained the composite materials of PVK grown on GO nanosheets for fabricating the nonvolatile resistance switching memory devices. The structures of the hybrid composite materials were analyzed by using transmission electron microscopy, atomic force microscopy, Fourier transform infrared spectroscopy and 13C-NMR spectroscopy. The film devices with the structure of Al/PVK-GO/PEDOT: PSS/ITO have been measured for the memory effects. The new devices exhibit the nonvolatile resistance switching effect with the ON/OFF current ratio as high as 104 at a read voltage of 1.0 V. Both the low resistance ON state and the high- resistance OFF state retain stable under a constant voltage stress for 104 s. The resistance-temperature dependence and current–voltage model studies are carried out for both OFF-state and ON-state. The resistance of the OFF state shows negative temperature dependence, indicating a typical semiconductor property. The resistance of the ON state increases with an increase in temperature, indicating a metallic behavior.
Co-reporter:Tiancheng Zheng and Xiuyuan Ni
RSC Advances 2016 vol. 6(Issue 62) pp:57122-57130
Publication Date(Web):27 May 2016
DOI:10.1039/C6RA08178A
Novel flame-resistant UV-curable epoxy (EP) composites were prepared using the organophosphorous flame retardant dimethyl methylphosphonate (DMMP) which was loaded into halloysite nanotubes (HNTs). We used a cone calorimeter to investigate the flame retardancy of the UV-curable epoxy resin containing DMMP-loaded halloysite nanotubes (HNT-D). It was found that compared with the neat epoxy resin the EP/HNT-D system exhibited better flame retardancy with an obvious decrease in the heat release rate (HRR), total heat release (THR), total smoke release (TSR), mass loss rate (MLR) and smoke production rate (SPR). Exploring the flame retardant mechanism revealed two reaction steps in the process of the flame retardant: DMMP gasification followed by a polyphosphoric-HNT carbon layer generating on the condensed phase. It was revealed through measuring the dynamic mechanical properties and tensile properties of the UV-cured EP materials that adding DMMP-loaded halloysite nanotubes (HNT-D) into EP obtained better mechanical properties than adding a simple mixture of halloysite clay and DMMP. With DMMP loaded in HNTs, the HNT-D could reduce the softening influence of DMMP. This method may potentially be applied to improve the flame retardancy of UV-curable epoxy resin in the future.
Co-reporter:Yongming Li and Xiuyuan Ni
RSC Advances 2016 vol. 6(Issue 20) pp:16340-16347
Publication Date(Web):02 Feb 2016
DOI:10.1039/C5RA25517A
Nonvolatile rewritable memory devices were fabricated from the composite films of poly(3,4-ethylenedioxythiophene) (PEDOT) grown on a graphene oxide (GO) substrate. Photopolymerization which used GO as the reaction initiator was carried out for preparing the GO–PEDOT composite films of the bilayer structure. The composite films were analyzed by specular reflection infrared spectroscopy, Raman, atomic force microscopy, field-emission scanning electron microscopy coupled with energy-dispersive X-ray analysis and thermogravimetric analysis. The electronic properties of the as-prepared GO–PEDOT composite films were revealed by solid-phase ultraviolet photoelectron spectroscopy and X-ray photoelectron spectroscopy. Fabricated from the composite films, the ITO/GO–PEDOT/Al device exhibits nonvolatile rewritable memory of high performance with an ON/OFF current ratio of 3 × 104 and turn-on voltage of 1.5 V. The current–voltage characteristics and resistance–temperature dependence at different resistance levels are discussed. The resistance of the OFF state presents negative temperature dependence, indicating a typical semiconductor property. The resistance of the ON state is found to increase with increasing temperature, indicating a metallic behavior.
Co-reporter:Jinrui Lin and Xiuyuan Ni
RSC Advances 2015 vol. 5(Issue 19) pp:14879-14886
Publication Date(Web):23 Jan 2015
DOI:10.1039/C4RA16079G
Two triarylamine-based polymers were synthesized by oxidative coupling reactions from 3-(N,N-diphenylamino) thiophene (3PAT) and 3-(10H-phenothiazin-10-yl) thiophene (3PTT) monomers, respectively. Distinguished from 3PAT, 3PTT has an additional sulfur atom between the two benzene rings. By using NMR spectroscopy and triarylamine control, the structures of the synthesized polymers were resolved with the aim of revealing the substitution effect. The results present that the substituent plays an important role in the chain propagation. Moreover, the triarylamine-based polymers were investigated for their solubility, thermal stability and electrochemical properties. To evaluate the electrochromism of the two different polymers, we have measured the spectroelectrochemical and electrochromic switching properties from the solution-cast films.
Co-reporter:Zongzhao Wei;Cheng Zou
Journal of Applied Polymer Science 2014 Volume 131( Issue 8) pp:
Publication Date(Web):
DOI:10.1002/app.40187
ABSTRACT
In this work, we prepare the TiO2 nanoparticle film and anatase TiO2 nanoarray film, and we achieve the polymerizations of thiophene using the photoexcited TiO2 film as the initiators. It is measured that the in situ polymerizations of thiophene take place on the surfaces of the two films. The growth of polythiophene (PTh) on the TiO2 nanoarray is monitored using Fourier-transform Raman spectroscopy. The TiO2 nanoarray is found to strongly interact with the PTh polymers. It is observed using scanning electron microscope that the microspores in the nanoarray are filled by the polymers after the reaction of 3 h, and the nanoarray is fully covered by the polymer layer when the polymerization lasts for 5 h. The PTh–TiO2 nanoarray composite films are measured for the transient photocurrents and photocurrent-voltage characteristics. The dependence of the photocurrents on the reaction time is revealed and discussed. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40187.
Co-reporter:Xun Ma and Xiuyuan Ni
Langmuir 2014 Volume 30(Issue 8) pp:2241-2248
Publication Date(Web):2017-2-22
DOI:10.1021/la404773r
We used the photoexcited TiO2 films to initiate the copolymerization of 3,4-ethylenedioxythiophene with pyrrole, aiming to develop an organic/inorganic heterojunction. Specular reflection infrared spectroscopy analysis was used to monitor the process of polymerization and indicated that the copolymers directly grew on the TiO2 substrate. Dissecting the copolymers with ultraviolet photoelectron spectroscopy revealed the evolution of the valence-band electronic structures. Moreover, the resulting copolymer/TiO2 heterojunctions were investigated using electrochemical impedence and X-ray photoelectron spectroscopy. The Al/poly(3,4-ethylenedioxythiophene-co-pyrrole)/TiO2/ITO heterojunction device that was prepared from the hybrid film exhibited a conspicuous rectification. The heterojunction device was also explored with respect to the conduction models.
Co-reporter:Feilong Li, Xiuyuan Ni
Solar Energy Materials and Solar Cells 2013 Volume 118() pp:109-115
Publication Date(Web):November 2013
DOI:10.1016/j.solmat.2013.08.012
•A heterojunction solar cell is prepared from poly (3-hexylthiophene) and the purposely surface-modified TiO2 nanorod array.•The modification is carried out by connecting polypyrrole to the TiO2 array through an in-situ photopolymerization.•The photovoltaic performances of the device are improved due to the surface modification.•The function of polypyrrole in the device is investigated by using electrochemical and intensity modulated photovoltage spectroscopes.A heterojunction solar cell is prepared from poly(3-hexylthiophene) (P3HT) and the purposely surface-modified TiO2 nanorod array. The modification is carried out by connecting polypyrrole (PPy) to the TiO2 nanorod array through an in-situ polymerization, which is initiated by photoexcited TiO2 nanorods. The as-prepared composite films are investigated by using photoluminescence emission spectroscopy, electrochemical impedance spectroscopy and intensity modulated photovoltage spectroscopy. The analysis results demonstrate that modifying TiO2 nanorod array with PPy increases the efficiency of charge separation and prolongs the electron lifetime. It is observed that the modified P3HT/PPy/TiO2 solar cell shows the power conversion efficiency which is 77% higher than that of the P3HT/TiO2 solar cell. These results prove that the in-situ photopolymerization is an efficient method to modify for the heterojunction solar cell.
Co-reporter:Zhouyong Yang and Xiuyuan Ni
Langmuir 2012 Volume 28(Issue 10) pp:4829-4834
Publication Date(Web):February 15, 2012
DOI:10.1021/la204990d
A new photovoltaic film consisting of monoclinic WO3 semiconductor and conjugated polythiophene (PT) is prepared via an in situ polymerization which is initiated by photoexcited WO3. It is observed that PT grows on the WO3 substrate along with reaction time, leading to uniform and high quality PT-WO3 composite films. Structures of the as-synthesized films are studied by using Raman and X-ray photoelectron spectroscopy (XPS) with the aim of gaining an insight into the interface. The results show that the sulfur sites of PT are bound to the semiconductor through a strong linkage and an acceptor–donor complex is formed as a result of the electron transfer from PT to WO3. The cyclic voltammetry analysis confirms the charge-transfer reaction. Film devices are fabricated by using the PT-WO3 composite film as the active layer and measured under AM 1.5G illumination for the photocurrents and incident photon-to-current conversion efficiency.
Co-reporter:Lihua Zhai, Zongzhao Wei, Zhouyong Yang, Xiuyuan Ni
Materials Letters 2010 Volume 64(Issue 4) pp:531-533
Publication Date(Web):28 February 2010
DOI:10.1016/j.matlet.2009.11.067
Hybrid composites of ZnS nanocrystals anchored on carbon nanotubes are prepared. Photochemical polymerization of acrylic acid is carried out using the ZnS nanocrystals as initiators. As a result of the surface polymerization, the modified CNT/ZnS hybrid composites are highly dispersed and the obtained solution exhibits long-term stability. In comparison, the synthesized poly(acrylic acid) exhibits higher thermal-stability. Investigations with Raman scattering reveal that ZnS nanocrystals interact with the carbon nanotubes, and the interaction is strengthened after UV irradiation. This study provides a new method to modify core–shell hybrid composites, and the obtained dispersible nanocomposites are useful for fabricating photoelectrical devices.
Co-reporter:Guowei Li, Guoquan Min, Licheng Fei, Xiuyuan Ni, Wenqi Lu
Journal of Colloid and Interface Science 2009 Volume 334(Issue 1) pp:8-12
Publication Date(Web):1 June 2009
DOI:10.1016/j.jcis.2009.03.003
This study designs a polymerization, in which ZnO colloids are used to initiate a copolymerization of N-vinylcarbazole and methyl acrylate, to synthesize functional composites for fabricating photoelectric devices. It is proved that a block copolymer is synthesized and a nanocomposite consisting of the ZnO and copolymer is obtained simultaneously. As a result, the ZnO nanocrystals are finely dispersed in the polymer matrix. A film-device is prepared from the obtained nanocomposite which has good film-forming ability and measured about photocurrents under illumination.ZnO colloids initiated copolymerization of N-vinylcarbazole (NVK) and methyl acrylate (MA). A nanocomposite consisting of the ZnO nanocrystals and copolymer was obtained.
Co-reporter:Zhen Weng, Xiuyuan Ni, Dan Yang, Jiao Wang, Weikang Chen
Journal of Photochemistry and Photobiology A: Chemistry 2009 Volume 201(2–3) pp:151-156
Publication Date(Web):25 January 2009
DOI:10.1016/j.jphotochem.2008.10.013
Polymerizations of vinyl acetate are photocatalyzed by TiO2 nanoparticles in presence of carboxylic acids including propionic acid, n-butyric acid and pivalic acid. Nuclear magnetic resonance (NMR) analysis using 13C-labeled n-butyric acid as the probing molecule demonstrates that the polymerization of vinyl acetate is initiated by alkyl radicals generated from photocatalytic decarboxylation of the carboxylic acid. A universal mechanism is established with extending the photo-Kolbe reaction from acetic acid to the carboxylic acids with longer chains. Kinetics studies find that n-butyric acid has higher initiation rate than acetic acid, indicating more efficient decarboxylation for butyric acid than acetic acid in their aqueous solutions. It is proved that carboxylates participate in the decarboxylation. Attenuated total reflection Fourier-transform infrared (ATR-FTIR) spectra are obtained with aqueous solutions of the carboxylic acids in contact with a layer of the TiO2 nanoparticles, and the observations are discussed with respect to the interaction between the TiO2 and carboxylic acids.
Co-reporter:Jiao Wang
Journal of Applied Polymer Science 2008 Volume 108( Issue 6) pp:3552-3558
Publication Date(Web):
DOI:10.1002/app.28020
Abstract
Poly(methyl methacrylate)/TiO2 nanocomposites have been prepared by the polymerization with photoexcited TiO2 nanoparticles as initiator. To reveal the interfacial structure, the composites obtained are investigated by FTIR and XPS analysis. The bound PMMA displays triply split IR bands attributed to the carbonyl stretching mode, meanwhile great changes also occur in the IR range closely related to the conformation of PMMA. Based on the area of the nonassociated and associated PMMA carbonyl stretching peaks in the FTIR spectrum, it is calculated out that the bound PMMA is constituted of 70% repeating units in nonassociated state and 30% units associated to TiO2 inorganic nanoparticles. Moreover, XPS analysis show that Ti2p doublet of the composites shift to lower binding energy by 1.0 eV, indicating the interaction between Ti atoms of TiO2 and oxygen atoms of PMMA. According to the observation that the interaction involves both carboxyl and carbonyl groups of PMMA, a bidentate complex is approved. In addition, compared with the extracted PMMA, certain backbone chains of bound PMMA have to change their rotational conformations from gauche to trans so as to bond to the surface active centers at TiO2 nanoparticles. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008
Co-reporter:Zhen Weng
Journal of Applied Polymer Science 2008 Volume 110( Issue 1) pp:109-116
Publication Date(Web):
DOI:10.1002/app.28636
Abstract
Oxidative polymerization of pyrrole is initiated by photoexcited TiO2 nanoparticles. Pyrrole oligomers and polypyrrole (PPy) are continuously produced with reaction time. The conversion of pyrrole monomer changes as a function of the concentration of TiO2 nanoparticles. It is found that PPy in the composite has the conjugated structure and is partially oxidized with a formation of positively charged N+. Results from X-ray photoelectron spectroscopy and Raman analysis consistently indicate that a strong interaction is established between the TiO2 and PPy. According to the results of UV–vis spectroscopy, a mechanism of photocatalytic oxidation is proposed for this polymerization. The interaction between TiO2 and PPy is found to arise from the photocatalytic reaction and discussed in terms of photoinduced Ti3+. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008
Co-reporter:Jiao Wang, Xiuyuan Ni
Solid State Communications 2008 Volume 146(5–6) pp:239-244
Publication Date(Web):May 2008
DOI:10.1016/j.ssc.2008.02.022
A Photosensitized electrode was fabricated through a novel polymerization of pyrrole initiated by TiO2 nanoparticles under UV irradiation. Conjugated polypyrrole (PPy) continuously grows on the surface of the TiO2 film, resulting in fully covered film with the stably-bound PPy layer. The film structures were analysed using Raman and X-ray photoelectron spectroscopy (XPS). It was found that the film electrode exhibits improved photoresponse including the flat band potential, photocurrent and separation of charges. The lowest unoccupied molecular orbital (LUMO) level of the PPy is higher in energy than the LUMO of PPy in electrodeposited electrodes, providing a stronger driving force for the electron injection into the TiO2.
Co-reporter:Xiuyuan Ni;Xiaohui Sun
Journal of Applied Polymer Science 2006 Volume 100(Issue 2) pp:879-885
Publication Date(Web):10 JAN 2006
DOI:10.1002/app.23012
Shape memory behaviors of trans-polyisoprene (TPI) segmented urethane copolymers were studied. Film specimens for cyclic loading tests were prepared from the polymer solution by casting, and tested at the loading temperature of 65°C. Results show that the recovery rates of the films depend on their TPI segment contents, while the fixity rate was measured to be close to 100% for each sample. The film containing 70% TPI segments was found to show a recovery rate of 85%. Two separated phases were clearly observed in the morphology of the films. The urethane segments were organized into spherical domains acting as physical cross-links during the shape memory process. The continuous phase formed by the crystalline TPI segments serves as the reversible phase responsible for fixation of the temporary shape. The tensile and dynamic thermal properties of those films were also studied. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 100: 879–885, 2006
Co-reporter:Xiuyuan Ni, Jing Ye, Ceng Dong
Journal of Photochemistry and Photobiology A: Chemistry 2006 Volume 181(Issue 1) pp:19-27
Publication Date(Web):5 July 2006
DOI:10.1016/j.jphotochem.2005.10.021
Kinetics of the photopolymerization of methyl methacrylate (MMA) initiated by TiO2 nanoparticles in aqueous suspensions was studied. The kinetics equation was established on basis of free radical chain mechanism. The observed dependences of polymerization rate on the variables of the concentration of TiO2 and the incident light intensity complied with the predictions from the kinetics equation. It was found that the polymerization rate as well as the number-average molecular weight of the synthetic polymers increased rapidly with increasing concentration of monomer. This phenomenon was explained by introducing a model of surface chain propagation. The effect of mass transfer was incorporated through addition of a diffusion flux term to the mass equilibrium of monomer. The initiation quantum efficiency was found to decrease with increasing incident light intensity. pH effects on the photopolymerization were investigated exclusively in this study. It was found that the rate of polymerization was pH dependent, while the configuration of polymer remains unchanged. The results from ESR spin-trapping analysis at various pH conditions suggested that trapping holes by OH− act as a competitive way towards OH radicals. With aids of these results, pH dependence of the initiation quantum efficiency was correlated to the influences of pH on the initiating species. Assuming that the photogenerated holes have higher initiation efficiency than OH radicals, the observed pH dependence of polymerization rate can be reasonably interpreted.
Co-reporter:Xiaohui Sun
Journal of Applied Polymer Science 2004 Volume 94(Issue 6) pp:2286-2294
Publication Date(Web):22 OCT 2004
DOI:10.1002/app.21016
A new type of urethane segmented copolymer was prepared from hydroxyl-terminated trans-polyisoprene (HTTPI) and toluene diisocyanate (TDI). The structures of the copolymer were characterized by FTIR and GPC. Crystalline properties of trans-polyisoprene (TPI) segments were investigated using WAXD and DSC techniques. The crystals of TPI segments are inclined to exist in low-melting form (LM). The melting temperature of TPI shifts to a lower temperature as the urethane segment was introduced. DMA studies show that, when TPI crystals were at the melting state, the storage modulus of the copolymer depended on the content of urethane segment. The hard segment here serves as physical crosslinkage. Nonisothermal crystallization kinetics of TPI segment was studied on the basis of the Ozawa equation. It was found that the hard segment suppresses the crystallization of the TPI segment. Morphology of two-phase separation was observed in the copolymer by SEM. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 94: 2286–2294, 2004
Co-reporter:Ni Xiuyuan, Hu Yuefang, Liu Bailin, Xu Xi
European Polymer Journal 2001 Volume 37(Issue 1) pp:201-206
Publication Date(Web):January 2001
DOI:10.1016/S0014-3057(00)00153-1
Ultrasonic degradation of hydroxyethyl cellulose (HEC) in aqueous solution was investigated. The degradation rate of this polymer was found to follow the Baramboim kinetic equation. Rate constants and the generating rates of radicals produced by ultrasonic irradiation were calculated, and the results showed their dependence on polymer concentration. Copolymers of methyl methacrylate/HEC and acrylic acid/HEC were prepared by ultrasound-induced polymerization. Biodegradability of the resultant polymers was assessed through enzymatic cellulase degradation tests. The two kinds of copolymers were found to be susceptible to the cellulase degradation.
Co-reporter:Feilong Li, Xiuyuan Ni
Solar Energy Materials and Solar Cells (November 2013) Volume 118() pp:109-115
Publication Date(Web):1 November 2013
DOI:10.1016/j.solmat.2013.08.012
•A heterojunction solar cell is prepared from poly (3-hexylthiophene) and the purposely surface-modified TiO2 nanorod array.•The modification is carried out by connecting polypyrrole to the TiO2 array through an in-situ photopolymerization.•The photovoltaic performances of the device are improved due to the surface modification.•The function of polypyrrole in the device is investigated by using electrochemical and intensity modulated photovoltage spectroscopes.A heterojunction solar cell is prepared from poly(3-hexylthiophene) (P3HT) and the purposely surface-modified TiO2 nanorod array. The modification is carried out by connecting polypyrrole (PPy) to the TiO2 nanorod array through an in-situ polymerization, which is initiated by photoexcited TiO2 nanorods. The as-prepared composite films are investigated by using photoluminescence emission spectroscopy, electrochemical impedance spectroscopy and intensity modulated photovoltage spectroscopy. The analysis results demonstrate that modifying TiO2 nanorod array with PPy increases the efficiency of charge separation and prolongs the electron lifetime. It is observed that the modified P3HT/PPy/TiO2 solar cell shows the power conversion efficiency which is 77% higher than that of the P3HT/TiO2 solar cell. These results prove that the in-situ photopolymerization is an efficient method to modify for the heterojunction solar cell.
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![2-Propenoic acid, 4-[1-(4-hydroxyphenyl)-1-methylethyl]phenyl ester](/data/chemimg/3781800/148861-70-5_b.png)
