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

Yixin Zhao, John R. Swierk, Jackson D. Megiatto, Benjamin Sherman, W. Justin Youngblood, Dongdong Qin, Deanna M. Lentz, Ana L Moore, Thomas A Moore, John Devens Gust, Thomas E. Mallouk

Research output: Contribution to journalArticle

202 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)15612-15616
Number of pages5
JournalProceedings of the National Academy of Sciences of the United States of America
Volume109
Issue number39
DOIs
Publication statusPublished - Sep 25 2012

Fingerprint

Biomimetics
Coloring Agents
Electrons
Water
Electrodes
Solar Energy
Light
Semiconductors
Photosystem II Protein Complex
Ruthenium
Histidine
Oxides
Genetic Recombination
Tyrosine
Hydrogen
Metals
Oxygen

Keywords

  • Artificial photosynthesis
  • Photoelectrochemistry

ASJC Scopus subject areas

  • General

Cite this

Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator. / Zhao, Yixin; Swierk, John R.; Megiatto, Jackson D.; Sherman, Benjamin; Youngblood, W. Justin; Qin, Dongdong; Lentz, Deanna M.; Moore, Ana L; Moore, Thomas A; Gust, John Devens; Mallouk, Thomas E.

In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 109, No. 39, 25.09.2012, p. 15612-15616.

Research output: Contribution to journalArticle

Zhao, Yixin ; Swierk, John R. ; Megiatto, Jackson D. ; Sherman, Benjamin ; Youngblood, W. Justin ; Qin, Dongdong ; Lentz, Deanna M. ; Moore, Ana L ; Moore, Thomas A ; Gust, John Devens ; Mallouk, Thomas E. / Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator. In: Proceedings of the National Academy of Sciences of the United States of America. 2012 ; Vol. 109, No. 39. pp. 15612-15616.
@article{1499e7533f3348df8f0299cf2d567452,
title = "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.",
keywords = "Artificial photosynthesis, Photoelectrochemistry",
author = "Yixin Zhao and Swierk, {John R.} and Megiatto, {Jackson D.} and Benjamin Sherman and Youngblood, {W. Justin} and Dongdong Qin and Lentz, {Deanna M.} and Moore, {Ana L} and Moore, {Thomas A} and Gust, {John Devens} and Mallouk, {Thomas E.}",
year = "2012",
month = "9",
day = "25",
doi = "10.1073/pnas.1118339109",
language = "English",
volume = "109",
pages = "15612--15616",
journal = "Proceedings of the National Academy of Sciences of the United States of America",
issn = "0027-8424",
number = "39",

}

TY - JOUR

T1 - Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator

AU - Zhao, Yixin

AU - Swierk, John R.

AU - Megiatto, Jackson D.

AU - Sherman, Benjamin

AU - Youngblood, W. Justin

AU - Qin, Dongdong

AU - Lentz, Deanna M.

AU - Moore, Ana L

AU - Moore, Thomas A

AU - Gust, John Devens

AU - Mallouk, Thomas E.

PY - 2012/9/25

Y1 - 2012/9/25

N2 - 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.

AB - 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.

KW - Artificial photosynthesis

KW - Photoelectrochemistry

UR - http://www.scopus.com/inward/record.url?scp=84866874701&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84866874701&partnerID=8YFLogxK

U2 - 10.1073/pnas.1118339109

DO - 10.1073/pnas.1118339109

M3 - Article

VL - 109

SP - 15612

EP - 15616

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

SN - 0027-8424

IS - 39

ER -