多级有序孔道结构氧化钛薄膜的合成及应用
文献类型：学位论文
| 作者 | 杜江 |
| 学位类别 | 博士 |
| 答辩日期 | 2012-05-21 |
| 授予单位 | 中国科学院研究生院 |
| 导师 | 王丹 |
| 关键词 | 二氧化钛 石墨烯 宏孔/介孔 光催化 |
| 其他题名 | Synthesis,Characterization and Property of TiO2 Based hierarchically-materials |
| 学位专业 | 化学工程 |
| 中文摘要 | 钛材料具有优越的光学、电学等性质，在光催化材料、染料敏化太阳能电池中的电极材料等知道其微观结构与光催化性质的关系；还将这种多级有序孔道结构的二氧化钛薄膜应用于染料敏化太阳能电池中。研究了具有Au@TiO2空心微球的制备和形成机理，实现了对其形貌和尺寸的调控，并将该二氧化钛纳米材料用于染料敏化太阳能电池的光阳极。多级有序的宏孔/介孔TiO2薄膜材料是通过三维有序排列的PS球以及表面活性剂P123为模板制备的。其中PS球模板用于形成宏孔结构，P123表面活性剂用于形成介孔结构。此外，还把石墨烯这种具体有良好电子接收能力以及电子传输能力的新型碳材料掺杂到该多级有序的TiO2薄膜中。由于宏孔结构的引入极大的提高了薄膜内部的物质传输速度，还有效缩短了薄膜中的介孔孔道长度，提高了薄膜有效比表面积。同时，石墨烯片层结构还有效地抑制了光生电子与空穴对的复合。光催化性质的研究结果表明，石墨烯掺杂的宏孔/介孔多级有序TiO2薄膜比TiO2介孔薄膜在光催化能力上有了显著的提升。研究了宏孔/介孔TiO2薄膜在DSSCs中的应用。制备出了宏孔/介孔TiO2薄膜和P25层复合的双层DSSCs薄膜电极。其中P25层采用手术刀法，将P25浆料刮涂至煅烧前包含模板的TiO2薄膜上，通过一次煅烧，制备出双层TiO2薄膜电极。其DSSCs光电转化效率的研究结果表明，宏孔/介孔TiO2薄膜层可以有效地增加薄膜电极对太阳光的散射，增加对染料的吸附量，提高电池的光电转化效率。和单层的P25薄膜电极的光电转化效率相比，双层薄膜电极的光电转化效率提升了约83%。利用水热法合成了Au@TiO2核壳纳米材料，并对该材料的合成机理、微观形貌调控进行了系统的研究。将其应用于DSSCs电极，研究了其光电转化性能。结果表明，利用Au@TiO2核壳结构材料构成的电极，太阳能电池光电转化效率可以达到8.13%，比传统的P25电极的光电转化效率提升约30% |
| 英文摘要 | Among various oxide semiconductor materials, titanium dioxide (TiO2) has been recognized as the most suitable material for widespread environmental applications because of its strong oxidizing power, low cost, high chemical inertness, and photostability. We have realized the hierarchically TiO2 film can grestly promote the performance in photocatalysis and dye-sensitized solar cells (DSSCs). The details are summarized as follows: Hierarchically ordered macro/mesoporous titania films have been produced through a confinement self-assembly method within the regular voids of a colloidal crystal with three-dimensional periodicity. Furthermore, graphene as an excellent electron-accepting and electron-transporting material has been incorporated into the hierarchically ordered macro/mesoporous titania frameworks by in situ reduction of graphene oxide added in the self-assembly system. Incorporation of interconnected macropores in mesoporous films improves the mass transport through the film, reduces the length of the mesopore channel, and increases the accessible surface area of the thin film, whereas the introduction of graphene effectively suppresses the charge recombination. Therefore, the significant enhancement of photocatalytic activity for degrading the methyl blue has been achieved. The apparent rate constants for macro/mesoporous titania films without and with grapheme are up to 0.045 and 0.071 min-1, respectively, almost 11 and 17 times higher than that for pure mesoporous titania films (0.0041 min-1). Hierarchically ordered macro-mesoporous TiO2 films (Ti-Ma-Me) were fabricated on fluorine-doped tin oxide (FTO) substrates through the confinement self-assembly method. The prepared Ti-Ma-Me possesses periodically ordered structure and a large specific surface area, which was applied as an interfacial layer between the nanocrystalline TiO2 film (P25-TiO2) and FTO electrode in the dye-sensitized solar cell (DSSC). The introduction of a Ti-Ma-Me interfacial layer increased the shortcircuit current density (Jsc) from 7.49 to 10.65 mA/cm2 and the open-circuit voltage (Voc) from 0.65 to 0.70 V as the result of its improved light harvesting efficiency by allowing for the high roughness factor and enhanced multiple internal reflection or scattering as well as reducing the back-transport reaction by blocking direct contact between the electrolyte and FTO electrode. Therefore, the photovoltaic conversion efficiency was improved by 83% from 3.04% to 5.55%, as compared to a device using a bare P25 TiO2 photoanode. Au@TiO2 hollow submicrospheres with controllable sizes and shell thicknesses are easily synthesized by the hydrothermal method. When Au@TiO2 hollow submicrospheres are used as the photoanodes of DSSCs, a power conversion efficiency of 8.13% is achieved, which exhibits a 30% increase compared with the conventional DSSCs fabricated with P25 TiO2 photoanodes. |
| 语种 | 中文 |
| 公开日期 | 2013-09-25 |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/1858]  |
| 专题 | 过程工程研究所_研究所（批量导入） |
| 推荐引用方式 GB/T 7714 | 杜江. 多级有序孔道结构氧化钛薄膜的合成及应用[D]. 中国科学院研究生院. 2012. |
入库方式： OAI收割
来源：过程工程研究所
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