Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells

Swierk, John R.; Méndez-Hernández, Dalvin D.; McCool, Nicholas S.; Liddell, Paul; Terazono, Yuichi; Pahk, Ian; Tomlin, John J.; Oster, Nolan V.; Moore, Thomas A.; Moore, Ana L.; Gust, Devens; Mallouk, Thomas E.

doi:10.1073/pnas.1414901112

Title: Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells

Journal Article · Mon Jan 12 00:00:00 EST 2015 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1414901112· OSTI ID:1235499

Swierk, John R. ^[1]; Méndez-Hernández, Dalvin D. ^[2]; McCool, Nicholas S. ^[1]; Liddell, Paul ^[2]; Terazono, Yuichi ^[2]; Pahk, Ian ^[2]; Tomlin, John J. ^[2]; Oster, Nolan V. ^[2]; Moore, Thomas A. ^[2]; Moore, Ana L. ^[2]; Gust, Devens ^[2]; Mallouk, Thomas E. ^[3]

Departments of aChemistry and
Department of Chemistry and Biochemistry and Center for Bio-Inspired Solar Fuel Production, Arizona State University, Tempe, AZ 85287
Departments of aChemistry and, Biochemistry and Molecular Biology, Pennsylvania State University, University Park, PA 16802, and

Solar fuel generation requires the efficient capture and conversion of visible light. In both natural and artificial systems, molecular sensitizers can be tuned to capture, convert, and transfer visible light energy. We demonstrate that a series of metal-free porphyrins can drive photoelectrochemical water splitting under broadband and red light (λ > 590 nm) illumination in a dye-sensitized TiO₂ solar cell. Here, we report the synthesis, spectral, and electrochemical properties of the sensitizers. Despite slow recombination of photoinjected electrons with oxidized porphyrins, photocurrents are low because of low injection yields and slow electron self-exchange between oxidized porphyrins. As a result, the free-base porphyrins are stable under conditions of water photoelectrolysis and in some cases photovoltages in excess of 1 V are observed.

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Research Organization:: Arizona State Univ., Tempe, AZ (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Solar Fuel Production (BISfuel)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-07ER15911; SC0001016; DGE1255832; ECS-0335765

OSTI ID:: 1235499

Alternate ID(s):: OSTI ID: 1348410

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 112 Journal Issue: 6; ISSN 0027-8424

Publisher:: Proceedings of the National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 127 works

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14 SOLAR ENERGY
36 MATERIALS SCIENCE
artificial photosynthesis
metal-free porphyrins
photoelectrochemical
visible light
water-splitting

Title: Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells

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