Proceedings of 6th International Conference on Hybrid and Organic Photovoltaics (HOPV14)
Publication date: 1st March 2014
Plasmonic core-shell Au@SiO2 nanoparticles incorporated into dye-sensitized solar cells (DSSCs) have recently been shown to enhance the overall efficiency of DSSCs.1 A thin silica coating on the gold cores is needed to provide better stability during thermal processing and improved chemical stability towards the corrosive electrolyte used in DSSCs, while it also can prevent quenching of the generated photo excitations.2 However, the thickness and completeness of the silica shell has proven crucial for the performance of the plasmonic particles and is largely controlled by the linking chemistry between the gold core and the silica shell.3 We have evaluated four different silica coating procedures of ~15 nm gold nanoparticles for usage in DSSCs.4 The chemical stability of these core-shell nanoparticles was assessed by dispersing the particles in iodide/triiodide electrolyte solution and the thermal stability by heating the particles up to 500 ºC. In order to maintain stable gold cores under these conditions, a complete silica coating was required, which was best obtained using (3-mercaptopropyl)trimethoxysilane (MPTMS) as a chemical linker between the gold surface and the SiO2 precursor. An incomplete SiO2 layer was obtained using (3-aminopropyl)trimethoxysilane (APTMS), which resulted in the dissolution of the gold core when exposed to the electrolyte (see figure below). The poor result observed for the APTMS sample can be explained by the relatively weak coordination of amine groups to the gold surface, which can lead to disorder at the core-shell interface and thus affect the shell formation. However, the resulting coating could be improved by using a subsequent Stöber reaction step. In situ TEM characterization indicated that the heating process only had minor effects on the core-shell structure as no deformation or cracking of the shell was observed. The final step was to evaluate how the stable Au@SiO2 nanoparticles were influencing a real DSSC device when mixed into the TiO2 photoanode. The plasmon-incorporated DSSCs showed ~10% increase in efficiency compared to devices without core-shell nanoparticles, while the IPCE spectrum revealed that the main enhancement of the device was located in the energy range close to the plasmon absorption peak of the gold nanoparticles (see figure below). The presented results further confirm the vast potential of using plasmonic particles to enhance the performance of DSSCs, but clearly also highlight the importance of a complete protective shell surrounding the metal core.
TEM images of synthesized core-shell nanoparticles with an incomplete silica coating (APTMS) and with a complete coating (MPTMS). Insets: Dispersions of the corresponding core-shell particles before and after iodide/triiodide electrolyte addition.
1 Brown, M. D.; Suutewong, T.; Sai, R.; Kumar, S.; D’Innocenzio, V.; Petrozza, A.; Lee, M. M.; Wiesner, U.; Snaith, H. J. Plasmonic Dye-Sensitized Solar Cells Using Core-Shell Metal-Insulator Nanoparticles. Nano Letters 2011, 11, 438-445.
2 Sheehan, S. W.; Noh, H.; Brudvig, G. W.; Cao, H.; Schmuttenmaer, C. A. Plasmonic Enhancement of Dye-Sensitized Solar Cells Using Core-Shell-Shell Nanostructures. Journal of Physical Chemistry C 2012, 117, 927-934.
3 Liz-Marzán, L. M.; Giersig, M.; Mulvaney, P. Synthesis of Nanosized Gold-Silica Core-Shell Particles. Langmuir 1996, 12, 4329-4335.
4 Törngren, B.; Akitsu, K.; Ylinen, A.; Sandén, S.; Jiang, H.; Ruokolainen, J.; Komatsu, M.; Hamamura, T.; Nakazaki, J.; Kubo, T.; Segawa, H.; Österbacka, R.; Smått, J. H. Investigation of Plasmonic Gold-Silica Core-Shell Nanoparticle Stability in Dye-Sensitized Solar Cell Applications, Journal of Colloid and Interface Science 2014, in press (doi: 10.1016/j.jcis.2013.11.085).
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