Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 112, Issue 6, Pages 1681-1686Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1414901112
Keywords
water-splitting; photoelectrochemical; metal-free porphyrins; visible light; artificial photosynthesis
Categories
Funding
- Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Energy Biosciences, Department of Energy [DE-FG02-07ER15911]
- Center for Bio-Inspired Solar Fuel Production, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001016]
- National Science Foundation (NSF) [DGE1255832]
- Pennsylvania State University Materials Research Institute Nanofabrication Laboratory under NSF [ECS-0335765]
- Direct For Education and Human Resources
- Division Of Graduate Education [0947962] Funding Source: National Science Foundation
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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 (lambda > 590 nm) illumination in a dye-sensitized TiO2 solar cell. 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. 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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