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    多孔性TiO2對CO2光催化還原特性探討研究
    (2008)
    張淑閔
    ;
    Sue-min Chang
    ;
    國立交通大學環境工程研究所
    光催化還原CO2 是現今非常受重視的溫室效應氣體處理技術，藉由光觸媒的電子在 能帶間的躍遷與表面轉移，可將光能轉換為化學能，使CO2 還原為高化學能的有機化 合物，提供清靜能源技術的燃料來源，然而CO2 光還原的產物包括CO、HCOOH、 HCHO、CH4 及CH3OH，其中僅CH3OH 與CH4 為熱值較高的燃料，因此提升光催化還 原CO2 的效率與產物選擇性是眾所努力的目標。許多研究指出TiO2 光觸媒能有效地以 H2O 為電子供給者，將CO2 光催化還原成CH3OH 與CH4，而觸媒的比表面積與微結構 決定光觸媒催化活性與產物選擇性，因此本研究創新地將結合模版溶膠-凝膠法與表面 溶膠-凝膠法製備高活性與高產物選擇性的表面金屬摻雜TiO2 光觸媒。首先以共聚合物 在溶膠溶液中形成的微胞為模版，經凝膠過程形成TiO2 後以鍛燒方式移除模版即可得 到高比表面積的中孔洞TiO2，爾後再以表面溶膠-凝膠法，將不同金屬離子(Si4+、Cu2+、 Fe3+與V5+)摻雜在TiO2 表面數個分子層的位置即形成中孔洞表面摻雜TiO2。此方法製 備出的中孔洞結構能提供大比表面積，同時骨架內的晶粒大小為能表現最大光催化活性 的尺寸(10-14 nm)，而表面摻雜物能降低電荷再結合機會，因此能大幅提昇CO2 光催化 還原效率，另外，表面摻雜物造成的氧缺陷能使H2O 更有效率地產生H 自由基而提高 CH3OH 產率。研究中將比較不同金屬摻雜物對TiO2 對光催化動力影響，同時最佳化光 催化還原系統的操作條件，最後分析中間產物與光觸媒反應前後表面微結構與化學組成 變化，配合比較不同催化條件下CO2 還原速率與產物物種分佈，提出CO2 光催化還原 機制，並釐清不同摻雜物、反應物物種與物種間比例對CO2 光催化反應動力與選擇性 的影響。預期本研究將能針對光催化還原CO2 提出高活性與高選擇性的光觸媒化學組 成與微結構組合，瞭解材料特性控制CO2 光催化還原反應的機制，並建立永續環保的 再生能源系統。
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    Item type:Item,
    多孔性TiO2對CO2光催化還原特性探討研究
    (2009)
    張淑閔
    ;
    Sue-min Chang
    ;
    國立交通大學環境工程研究所
    光催化還原CO2 是現今非常受重視的溫室效應氣體處理技術，藉由光觸媒的電子在 能帶間的躍遷與表面轉移，可將光能轉換為化學能，使CO2 還原為高化學能的有機化 合物，提供清靜能源技術的燃料來源，然而CO2 光還原的產物包括CO、HCOOH、 HCHO、CH4 及CH3OH，其中僅CH3OH 與CH4 為熱值較高的燃料，因此提升光催化還 原CO2 的效率與產物選擇性是眾所努力的目標。許多研究指出TiO2 光觸媒能有效地以 H2O 為電子供給者，將CO2 光催化還原成CH3OH 與CH4，而觸媒的比表面積與微結構 決定光觸媒催化活性與產物選擇性，因此本研究創新地將結合模版溶膠-凝膠法與表面 溶膠-凝膠法製備高活性與高產物選擇性的表面金屬摻雜TiO2 光觸媒。首先以共聚合物 在溶膠溶液中形成的微胞為模版，經凝膠過程形成TiO2 後以鍛燒方式移除模版即可得 到高比表面積的中孔洞TiO2，爾後再以表面溶膠-凝膠法，將不同金屬離子(Si4+、Cu2+、 Fe3+與V5+)摻雜在TiO2 表面數個分子層的位置即形成中孔洞表面摻雜TiO2。此方法製 備出的中孔洞結構能提供大比表面積，同時骨架內的晶粒大小為能表現最大光催化活性 的尺寸(10-14 nm)，而表面摻雜物能降低電荷再結合機會，因此能大幅提昇CO2 光催化 還原效率，另外，表面摻雜物造成的氧缺陷能使H2O 更有效率地產生H 自由基而提高 CH3OH 產率。研究中將比較不同金屬摻雜物對TiO2 對光催化動力影響，同時最佳化光 催化還原系統的操作條件，最後分析中間產物與光觸媒反應前後表面微結構與化學組成 變化，配合比較不同催化條件下CO2 還原速率與產物物種分佈，提出CO2 光催化還原 機制，並釐清不同摻雜物、反應物物種與物種間比例對CO2 光催化反應動力與選擇性 的影響。預期本研究將能針對光催化還原CO2 提出高活性與高選擇性的光觸媒化學組 成與微結構組合，瞭解材料特性控制CO2 光催化還原反應的機制，並建立永續環保的 再生能源系統。
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    Enhanced charge transfer character of photoexcited states of dye sensitizer on the N719/TiO2 interface as revealed by electroabsorption spectra
    (2014-08-15)
    Awasthi, Kamlesh
    ;
    Hsu, Hung-Yu
    ;
    Diau, Eric Wei-Guang
    ;
    Ohta, Nobuhiro
    ;
    應用化學系
    Electroabsorption (E-A) spectra of (Bu4N)(2)[Ru(dcbpyH)(2)(NCS)(2)] (N719) sensitized on TiO2 nanoparticles are very different from those of the N719 solid film. In contrast with N719 fixed in a solid form, N719 adsorbed on TiO2 shows a significant electric field effect on absorbance, indicating the strong interaction in the surface between N719 and TiO2. The magnitude of the change in electric dipole moment following absorption of N719 sensitized on TiO2 is much greater than that of the sold film, suggesting that the interfacial charge transfer occurs following photoexcitation of N719 adsorbed on TiO2 surface. (C) 2014 Elsevier B.V. All rights reserved.
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    Revealing Controllable Nanowire Transformation through Cationic Exchange for RRAM Application
    (2014-05-01)
    Huang, Chun-Wei
    ;
    Chen, Jui-Yuan
    ;
    Chiu, Chung-Hua
    ;
    Wu, Wen-Wei
    ;
    材料科學與工程學系
    One dimensional metal oxide nanostructures have attracted much attention owing to their fascinating functional properties. Among them, piezoelectricity and photocatalysts along with their related materials have stirred significant interests and widespread studies in recent years. In this work, we successfully transformed piezoelectric ZnO into photocatalytic TiO2 and formed TiO2/ZnO axial heterostructure nanowires with flat interfaces by solid to solid cationic exchange reactions in high vacuum (approximately 10(-8) Torr) transmission electron microscope (TEM). Kinetic behavior of the single crystalline TiO2 was systematically analyzed. The nanoscale growth rate of TiO2 has been measured using in situ TEM videos. On the basis of the rate, we can control the dimensions of the axial-nanoheterostructure. In addition, the unique Pt/ ZnO / TiO2/ ZnO /Pt heterostructures with complementary resistive switching (CRS) characteristics were designed to solve the important issue of sneak-peak current. The resistive switching behavior was attributed to the migration of oxygen and TiO2 layer served as reservoir, which was confirmed by energy dispersive spectrometry (EDS) analysis. This study not only supplied a distinct method to explore the transformation mechanisms but also exhibited the potential application of ZnO/TiO2 heterostructure in nanoscale crossbar array resistive random-access memory (RRAM).
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    The structure, electronic, and optical properties of (Sm,N)-codoped anatase TiO2 photocatalyst: A density functional study
    (2014-01-01)
    Lin, Yanming
    ;
    Jiang, Zhenyi
    ;
    Zhang, Ruiqin
    ;
    Zhu, Chaoyuan
    ;
    Hu, Xiaoyun
    The geometrical, electronic, and optical properties of Sm-doped, N-doped, and (Sm,N)-codoped anatase TiO2 were successfully calculated and simulated using the spin-polarized density functional theory. The researches of geometrical structures show that (Sm,N) codoping leads to lattice distortion, which reduces the recombination of the photogenerated electron-hole pairs. Moreover, the calculated results indicate that the synergistic effects of (Sm,N) codoping can lead to an obvious band gap narrowing and a N 2p state appearing in the forbidden gap, which leads to a significant redshift of the optical absorption edge and enhances the photocatalytic activity of the (Sm,N)-codoped anatase TiO2. (C) 2013 Elsevier Inc. All rights reserved.
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    Low power resistive random access memory using interface-engineered dielectric stack of SiOx/a-Si/TiOy with 1D1R-like structure
    (2014-01-01)
    Cheng, Chun-Hu
    ;
    Chou, K. I.
    ;
    Zheng, Zhi-Wei
    ;
    Hsu, Hsiao-Hsuan
    ;
    電子工程學系及電子研究所
    In this study, we report a resistive random access memory (RRAM) using trilayer SiOx/a-Si/TiOy film structure. The low switching energy of <10 pJ, highly uniform current distribution (<13% variation), fast 50-ns speed and stable cycling endurance for 10(6) cycles are simultaneously achieved in this RRAM device. Such good performance can be ascribed to the use of interface-engineered dielectric stack with 1D1R-like structure. The SiOx tunnel barrier in contact with top Ni electrode to form diode-like rectifying element not only lowers self-compliance switching currents, but also improves cycling endurance, which is favorable for the application of high-density 3D memory. (C) 2013 Elsevier B. V. All rights reserved.
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    High Mobility Bilayer Metal-Oxide Thin Film Transistors Using Titanium-Doped InGaZnO
    (2014-01-01)
    Hsu, Hsiao-Hsuan
    ;
    Chang, Chun-Yen
    ;
    Cheng, Chun-Hu
    ;
    Chiou, Shan-Haw
    ;
    Huang, Chiung-Hui
    We report a high performance indium-gallium-zinc oxide (IGZO)/IGZO:Ti bilayer metal-oxide thin-film transistor (TFT) with a low drive voltage of <2 V. Compared with conventional IGZO TFTs, the novel bilayer metal-oxide TFTs through IGZO thickness modulation can reach the lowest off current of 1.6 x 10(-11) A, smallest sub-threshold swing of 73 mV/decade, and highest mobility of 63 cm(2)/Vs, which may create the potential application for high resolution display.
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    Fully room-temperature IGZO thin film transistors adopting stacked gate dielectrics on flexible polycarbonate substrate
    (2013-11-01)
    Hsu, Hsiao-Hsuan
    ;
    Chang, Chun-Yen
    ;
    Cheng, Chun-Hu
    ;
    Yu, Shu-Hung
    ;
    Su, Ching-Yuan
    This study demonstrates the feasibility of producing an InGaZnO thin-film transistor (TFT) using a high-kappa germanium oxide (GeO2)/titanium oxide (TiO2)/GeO2 gate stack on a flexible polycarbonate substrate. The flexible TFT exhibited a small sub-threshold swing of 0.132 V/decade, an acceptable field effect mobility of 8 cm(2)/(V s), and a robust I-on/I-off ratio of 2.4 x 10(7). The improved device performance can be attributed to the combined effect of high-kappa TiO2 and the large band gap of GeO2 that exhibits a tendency to remain in a Ge4+ oxidation state at room temperature. (C) 2013 Elsevier Ltd. All rights reserved.
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    Electronic and optical performances of Si and Fe-codoped TiO2 nanoparticles: A photocatalyst for the degradation of methylene blue
    (2013-10-01)
    Lin, Yanming
    ;
    Jiang, Zhenyi
    ;
    Zhu, Chaoyuan
    ;
    Hu, Xiaoyun
    ;
    Zhang, Xiaodong
    The effect of substitutional Si, Fe, and Si and Fe (co)doping on the electronic structure and optical properties of anatase and rutile TiO2 have been investigated by the density functional theory. The calculated results indicate that Si doping TiO2 will induce an obvious band gap narrowing by mixing O 2p with Si 3p states, and a series of impurity energy levels (Fe 3d) appear in edge of the VB and the CB through Fe doping. The synergistic effects of Si and Fe codoping can extend optical absorption edge, which leads to higher visible-light photocatalytic activities than pure and monodoped anatase TiO2. Si and Fe-codoped TiO2 nanoparticles was prepared by a sol-gel-solvothermal method, and the photocatalytic activity of TiO2 nanoparticles was examined by measuring the rate of methylene blue decomposition. The experimental results show that Si and Fe-codoped TiO2 sample exhibits better optical absorption performance and higher photocatalytic activities for the degradation of methylene blue than pure and monodoped TiO2, which verifies the reliability of our calculated results. (c) 2013 Elsevier B.V. All rights reserved.
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    Au Nanostructure-Decorated TiO2 Nanowires Exhibiting Photoactivity Across Entire UV-visible Region for Photoelectrochemical Water Splitting
    (2013-08-01)
    Pu, Ying-Chih
    ;
    Wang, Gongming
    ;
    Chang, Kao-Der
    ;
    Ling, Yichuan
    ;
    Lin, Yin-Kai
    Here we demonstrate that the photoactivity of Au-decorated TiO2 electrodes for photoelectrochemical water oxidation can be effectively enhanced in the entire UV-visible region from 300 to 800 nm by manipulating the shape of the decorated Au nanostructures. The samples were prepared by carefully depositing Au nanoparticles (NPs), Au nanorods (NRs), and a mixture of Au NPs and NRs on the surface of TiO2 nanowire arrays. As compared with bare TiO2, Au NP-decorated TiO2 nanowire electrodes exhibited significantly enhanced photoactivity in both the UV and visible regions. For Au NR-decorated TiO2 electrodes, the photoactivity enhancement was, however, observed in the visible region only, with the largest photocurrent generation achieved at 710 nm. Significantly, TiO2 nanowires deposited with a mixture of Au NPs and NRs showed enhanced photoactivity in the entire UV visible region. Monochromatic incident photon-to-electron conversion efficiency measurements indicated that excitation of surface plasmon resonance of Au is responsible for the enhanced photoactivity of Au nanostructure-decorated TiO2 nanowires. Photovoltage experiment showed that the enhanced photoactivity of Au NP-decorated TiO2 in the UV region was attributable to the effective surface passivation of Au NPs. Furthermore, 3D finite-difference time domain simulation was performed to investigate the electrical field amplification at the interface between Au nanostructures and TiO2 upon SPR excitation. The results suggested that the enhanced photoactivity of Au NP-decorated TiO2 in the UV region was partially due to the increased optical absorption of TiO2 associated with SPR electrical field amplification. The current study could provide a new paradigm for designing plasmonic metal/semiconductor composite systems to effectively harvest the entire UV visible light for solar fuel production.