Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator

Authors: Zhao, Y., Swierk, J. R., Megiatto, J. D., Sherman, B., Youngblood, W. J., Qin, D., Lentz, D. M., Moore, A. L., Moore, T. A., Gust, D., and Mallouk, T. E.
Title: Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator
Source: Proceedings of the National Academy of Sciences
Year: 2012
Volume: 109
Pages: 15612-15616

ABSTRACT:

Photoelectrochemical water splitting directly converts solar energy to chemical energy stored in hydrogen, a high energy density fuel. Although water splitting using semiconductor photoelectrodes has been studied for more than 40 years, it has only recently been demonstrated using dye-sensitized electrodes. The quantum yield for water splitting in these dye-based systems has, so far, been very low because the charge recombination reaction is faster than the catalytic four-electron oxidation of water to oxygen. We show here that the quantum yield is more than doubled by incorporating an electron transfer mediator that is mimetic of the tyrosine-histidine mediator in Photosystem II. The mediator molecule is covalently bound to the water oxidation catalyst, a colloidal iridium oxide particle, and is coadsorbed onto a porous titanium dioxide electrode with a Ruthenium polypyridyl sensitizer. As in the natural photosynthetic system, this molecule mediates electron transfer between a relatively slow metal oxide catalyst that oxidizes water on the millisecond timescale and a dye molecule that is oxidized in a fast light-induced electron transfer reaction. The presence of the mediator molecule in the system results in photoelectrochemical water splitting with an internal quantum efficiency of approximately 2.3% using blue light.


Date of online publication: Mon, 2012-04-30
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