Center for Nano Science and Technology@PoliMi, Istituto Italiano di Tecnologia , Via Giovanni Pascoli, 70/3, 20133 Milano, Italy.
ACS Nano. 2013 Nov 26;7(11):10023-31. doi: 10.1021/nn403979h. Epub 2013 Nov 7.
In this work we demonstrate hyperbranched nanostructures, grown by pulsed laser deposition, composed of one-dimensional anatase single crystals assembled in arrays of high aspect ratio hierarchical mesostructures. The proposed growth mechanism relies on a two-step process: self-assembly from the gas phase of amorphous TiO2 clusters in a forest of tree-shaped hierarchical mesostructures with high aspect ratio; oriented crystallization of the branches upon thermal treatment. Structural and morphological characteristics can be optimized to achieve both high specific surface area for optimal dye uptake and broadband light scattering thanks to the microscopic feature size. Solid-state dye sensitized solar cells fabricated with arrays of hyperbranched TiO2 nanostructures on FTO-glass sensitized with D102 dye showed a significant 66% increase in efficiency with respect to a reference mesoporous photoanode and reached a maximum efficiency of 3.96% (among the highest reported for this system). This result was achieved mainly thanks to an increase in photogenerated current directly resulting from improved light harvesting efficiency of the hierarchical photoanode. The proposed photoanode overcomes typical limitations of 1D TiO2 nanostructures applied to ss-DSC and emerges as a promising foundation for next-generation high-efficiency solid-state devices comprosed of dyes, polymers, or quantum dots as sensitizers.
在这项工作中,我们展示了通过脉冲激光沉积生长的超支化纳米结构,由一维锐钛矿单晶组装在高纵横比的分级介孔结构的阵列中组成。所提出的生长机制依赖于两步过程:在具有高纵横比的树状分级介孔结构的森林中,从气相自组装无定形 TiO2 团簇;在热处理时,支链的定向结晶。通过微观特征尺寸,可以优化结构和形态特征,以实现高比表面积以获得最佳染料吸收和宽带光散射。在 FTO 玻璃上用 D102 染料敏化的阵列中制造的固态染料敏化太阳能电池,与参考介孔光电阳极相比,效率提高了 66%,达到了 3.96%的最大效率(在该系统中报道的最高效率之一)。这一结果主要得益于分层光电阳极的光捕获效率的提高,从而直接增加了光生电流。所提出的光电阳极克服了应用于 ss-DSC 的一维 TiO2 纳米结构的典型限制,并为下一代高效率的固态器件奠定了基础,这些器件由染料、聚合物或量子点作为敏化剂组成。