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


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.

SUBMITTER: Zhao Y 

PROVIDER: S-EPMC3465399 | biostudies-literature | 2012 Sep

REPOSITORIES: biostudies-literature

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

Zhao Yixin Y   Swierk John R JR   Megiatto Jackson D JD   Sherman Benjamin B   Youngblood W Justin WJ   Qin Dongdong D   Lentz Deanna M DM   Moore Ana L AL   Moore Thomas A TA   Gust Devens D   Mallouk Thomas E TE  

Proceedings of the National Academy of Sciences of the United States of America 20120430 39


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 w  ...[more]

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