量子点敏化TiO_2基纳米结构太阳能电池制备与表征
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摘要
量子点敏化太阳能电池(Quantum dots sensitized solar cells)是目前材料科学、物理、化学等交叉学科的热点研究方向,国外学者预测该类电池是未来高效率低成本太阳电池的最佳候选之一。但是迄今光电转换效率还无法与染料敏化太阳能电池相媲美是制约该种电池进一步发展的瓶颈。基于目前国内外量子点敏化电池的研究进展,本论文结合已经成熟的纳米薄膜制备工艺,对改善量子点敏化电池的光电转换效率进行了系列探索研究。主要结果与创新点如下：
1、制备了CdS量子点敏化Ti02纳米晶多孔薄膜太阳能电池,发现通过提高工作电极孔隙率,可改善CdS量子点对其“浸润”性修饰；以“整体烧结”方式在FTO导电玻璃与Ti02纳米晶多孔薄膜之间引入Ti02致密层可改善其界面接触；采用ZnS层钝化CdS量子点可以提高电池的短路电流密度,电池的光电转换效率可达1.84%；电池经高压汞灯持续照射168 h,性能稳定,光电转换效率仅下降5%。
2、以镀有Sn02晶种层的玻璃基片为原始衬底,通过控制晶种层的表面粗糙度和外露晶面,并引入离子屏蔽剂,利用水热法成功制备了可剥离的无支撑金红石型Ti02纳米棒阵列薄膜。移植到导电玻璃上将其作为CdS量子点敏化太阳能电池的工作电极,经ZnS钝化后电池光电转换效率达到1.27%。
3、利用溶剂热法以Ti片为Ti源生长纳米棒阵列,利用CH30H/Br2混合溶液腐蚀剩余Ti片,成功制备出无支撑锐钛矿型TiO2纳米阵列薄膜。移植到导电玻璃上作为CdS量子点敏化太阳能电池的工作电极,经ZnS钝化后电池光电转换效率为1.55%。
4、利用快速热注入法在油胺体系中,通过控制反应速率,成功制备了分别具有黄铜矿、闪锌矿和纤锌矿三种不同晶型的单分散CuInS2量子点,结果表明,较快的反应速率有利于得到黄铜矿结构CuInS2量子点,反之则得到闪锌矿或纤锌矿结构的CuInS2量子点。该类量子点几乎可吸收全部可见光区的太阳光。
5、采用二次阳极氧化法成功制备出两端开孔无支撑Ti02纳米管阵列薄膜,二次阳极氧化的脉冲电压上限幅值越大,阵列薄膜底部开孔率越高；将无支撑Ti02纳米管阵列薄膜移植到导电玻璃上作为工作电极,试制了新型结构CuInS2量子点敏化太阳能电池,经ZnS钝化后,其光电转换效率为0.64%。
Quantum dots-sensitized solar cell (QDSSC) is one of the hottest spotlights as the crossdisciplinary research of materials science, physics, and chemistry. Many researchers have forecasted that these devices will be one of the most potential photovoltaics with high-efficiency and low-cost. However, the lower power conversion efficiency which can't compete with that of DSSCs has still been the "bottleneck" for limiting their further development. Based on the recent progress of QDSSC's researches, the exploratory researches were performed on the QDSSC, especially for improving their power conversion efficiency by combining the well-established preparation technologies on the nano-structured fim. The main results and conclusions are summarized as follows:
Firstly, a series of CdS quantum dots-sensitized TiO2 nanoparticulate film solar cells were prepared. It was found that the CdS QDs well-covered working electrode can be obtained by increasing the porosity of TiO2 film; the interface contactance of a compact TiO2 layer between FTO substrate and TiO2 working electrode can be improved by sintering the compact layer together with the electrode; after passivated by ZnS layer, the short current density (Jsc) of the CdS QDs sensitized TiO2 solar cells can be improved, with the power conversion efficiency of 1.84%. The solar cell shows good stability after the irradiation of high-voltage mercury lamp for 168 hours, the power conversion efficiency drops as little as for 5%.
Secondly, free-standing TiO2 (rutile) nanorod arrays films were successfully prepared by hydrothermal method using the silde glass coated with SnO2 seed layer as the original substrate, through the control of surface texture and exposed crystalline plane of SnO2 and the introduction of screening agent. The obtained free-standing film was transplanted onto FTO glass to fabricate the working electrode for CdS quantum dots-sensitized solar cells. After the passivation with ZnS, the solar cells based on the corresponding working electrode exhibited photo-to-current efficiency of 1.27%.
Thirdly, free-standing anatase TiO2 nanorod arrays films were successfully prepared through solvothermal method by using commercial Ti foils as the Ti source and substrate for growth of TiO2 nanorods and using the mixed Br2/CH3OH solution to etch the residual Ti substrate. The obtained free-standing film was transplanted onto FTO glass to fabricate the working electrode for CdS quantum dots-sensitized solar cells. After the passivation with ZnS, the solar cells based on the corresponding working electrode exhibited photo-to-current efficiency of 1.55%.
Fourthly, mono-disperse CuInS2 quantum dots with three different types of crystal structure (including chalcopyrite, zinc-blende and wurtzite) were successfully synthesized in oleylamine reaction system via hot-injection method by controlling the reaction rate of the system. It was indicated that the higher reaction rate is propitious to obtain chalcopyrite-structural CuInS2 quantum dots, otherwise, CuInS2 quantum dots with zinc-blende or wurtzite structure will be obtained. The CuInS2 quantum dots can absorb almost the all of visible light.
Fifthly, free-standing TiO2 nano-tubes array films with both-end opened are successfully prepared by the two-step anodic oxidations. During the second anodic oxidation, the larger maximum the amplitude of impulsive voltage applied to, the higher percentage of bottom-open tubes area of the free-standing film exhibited. The obtained free-standing TiO2 nano-tubes array films were transplanted onto FTO glass to fabricate the working electrodes, and a novel structure of CuInS2 quantum dots sensitized solar cells were developed tentatively. After the passivation with ZnS, the solar cells based on the corresponding working electrode exhibited photo-to-current efficiency of 0.64%.
1、制备了CdS量子点敏化Ti02纳米晶多孔薄膜太阳能电池,发现通过提高工作电极孔隙率,可改善CdS量子点对其“浸润”性修饰；以“整体烧结”方式在FTO导电玻璃与Ti02纳米晶多孔薄膜之间引入Ti02致密层可改善其界面接触；采用ZnS层钝化CdS量子点可以提高电池的短路电流密度,电池的光电转换效率可达1.84%；电池经高压汞灯持续照射168 h,性能稳定,光电转换效率仅下降5%。
2、以镀有Sn02晶种层的玻璃基片为原始衬底,通过控制晶种层的表面粗糙度和外露晶面,并引入离子屏蔽剂,利用水热法成功制备了可剥离的无支撑金红石型Ti02纳米棒阵列薄膜。移植到导电玻璃上将其作为CdS量子点敏化太阳能电池的工作电极,经ZnS钝化后电池光电转换效率达到1.27%。
3、利用溶剂热法以Ti片为Ti源生长纳米棒阵列,利用CH30H/Br2混合溶液腐蚀剩余Ti片,成功制备出无支撑锐钛矿型TiO2纳米阵列薄膜。移植到导电玻璃上作为CdS量子点敏化太阳能电池的工作电极,经ZnS钝化后电池光电转换效率为1.55%。
4、利用快速热注入法在油胺体系中,通过控制反应速率,成功制备了分别具有黄铜矿、闪锌矿和纤锌矿三种不同晶型的单分散CuInS2量子点,结果表明,较快的反应速率有利于得到黄铜矿结构CuInS2量子点,反之则得到闪锌矿或纤锌矿结构的CuInS2量子点。该类量子点几乎可吸收全部可见光区的太阳光。
5、采用二次阳极氧化法成功制备出两端开孔无支撑Ti02纳米管阵列薄膜,二次阳极氧化的脉冲电压上限幅值越大,阵列薄膜底部开孔率越高；将无支撑Ti02纳米管阵列薄膜移植到导电玻璃上作为工作电极,试制了新型结构CuInS2量子点敏化太阳能电池,经ZnS钝化后,其光电转换效率为0.64%。
Quantum dots-sensitized solar cell (QDSSC) is one of the hottest spotlights as the crossdisciplinary research of materials science, physics, and chemistry. Many researchers have forecasted that these devices will be one of the most potential photovoltaics with high-efficiency and low-cost. However, the lower power conversion efficiency which can't compete with that of DSSCs has still been the "bottleneck" for limiting their further development. Based on the recent progress of QDSSC's researches, the exploratory researches were performed on the QDSSC, especially for improving their power conversion efficiency by combining the well-established preparation technologies on the nano-structured fim. The main results and conclusions are summarized as follows:
Firstly, a series of CdS quantum dots-sensitized TiO2 nanoparticulate film solar cells were prepared. It was found that the CdS QDs well-covered working electrode can be obtained by increasing the porosity of TiO2 film; the interface contactance of a compact TiO2 layer between FTO substrate and TiO2 working electrode can be improved by sintering the compact layer together with the electrode; after passivated by ZnS layer, the short current density (Jsc) of the CdS QDs sensitized TiO2 solar cells can be improved, with the power conversion efficiency of 1.84%. The solar cell shows good stability after the irradiation of high-voltage mercury lamp for 168 hours, the power conversion efficiency drops as little as for 5%.
Secondly, free-standing TiO2 (rutile) nanorod arrays films were successfully prepared by hydrothermal method using the silde glass coated with SnO2 seed layer as the original substrate, through the control of surface texture and exposed crystalline plane of SnO2 and the introduction of screening agent. The obtained free-standing film was transplanted onto FTO glass to fabricate the working electrode for CdS quantum dots-sensitized solar cells. After the passivation with ZnS, the solar cells based on the corresponding working electrode exhibited photo-to-current efficiency of 1.27%.
Thirdly, free-standing anatase TiO2 nanorod arrays films were successfully prepared through solvothermal method by using commercial Ti foils as the Ti source and substrate for growth of TiO2 nanorods and using the mixed Br2/CH3OH solution to etch the residual Ti substrate. The obtained free-standing film was transplanted onto FTO glass to fabricate the working electrode for CdS quantum dots-sensitized solar cells. After the passivation with ZnS, the solar cells based on the corresponding working electrode exhibited photo-to-current efficiency of 1.55%.
Fourthly, mono-disperse CuInS2 quantum dots with three different types of crystal structure (including chalcopyrite, zinc-blende and wurtzite) were successfully synthesized in oleylamine reaction system via hot-injection method by controlling the reaction rate of the system. It was indicated that the higher reaction rate is propitious to obtain chalcopyrite-structural CuInS2 quantum dots, otherwise, CuInS2 quantum dots with zinc-blende or wurtzite structure will be obtained. The CuInS2 quantum dots can absorb almost the all of visible light.
Fifthly, free-standing TiO2 nano-tubes array films with both-end opened are successfully prepared by the two-step anodic oxidations. During the second anodic oxidation, the larger maximum the amplitude of impulsive voltage applied to, the higher percentage of bottom-open tubes area of the free-standing film exhibited. The obtained free-standing TiO2 nano-tubes array films were transplanted onto FTO glass to fabricate the working electrodes, and a novel structure of CuInS2 quantum dots sensitized solar cells were developed tentatively. After the passivation with ZnS, the solar cells based on the corresponding working electrode exhibited photo-to-current efficiency of 0.64%.
引文
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