Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers

Abstract A conductive polymer (poly(p-phenylenevinylene), PPV) was covalently modified with RuII complexes to develop an all-polymer photocathode as a conceptual alternative to dye-sensitized NiO, which is the current state-of-the-art photocathode in solar fuels research. Photocathodes require effic...

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Autores principales:	Ruri A. Wahyuono, Bianca Seidler, Sebastian Bold, Andrea Dellith, Jan Dellith, Johannes Ahner, Pascal Wintergerst, Grace Lowe, Martin D. Hager, Maria Wächtler, Carsten Streb, Ulrich S. Schubert, Sven Rau, Benjamin Dietzek
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/9a04f15eb5e3486d934ccb2afd9c3d19
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spelling	oai:doaj.org-article:9a04f15eb5e3486d934ccb2afd9c3d192021-12-02T14:06:49ZPhotocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers10.1038/s41598-021-82395-x2045-2322https://doaj.org/article/9a04f15eb5e3486d934ccb2afd9c3d192021-02-01T00:00:00Zhttps://doi.org/10.1038/s41598-021-82395-xhttps://doaj.org/toc/2045-2322Abstract A conductive polymer (poly(p-phenylenevinylene), PPV) was covalently modified with RuII complexes to develop an all-polymer photocathode as a conceptual alternative to dye-sensitized NiO, which is the current state-of-the-art photocathode in solar fuels research. Photocathodes require efficient light-induced charge-transfer processes and we investigated these processes within our photocathodes using spectroscopic and spectro-electrochemical techniques. Ultrafast hole-injection dynamics in the polymer were investigated by transient absorption spectroscopy and charge transfer at the electrode–electrolyte interface was examined with chopped-light chronoamperometry. Light-induced hole injection from the photosensitizers into the PPV backbone was observed within 10 ps and the resulting charge-separated state (CSS) recombined within ~ 5 ns. This is comparable to CSS lifetimes of conventional NiO-photocathodes. Chopped-light chronoamperometry indicates enhanced charge-transfer at the electrode–electrolyte interface upon sensitization of the PPV with the RuII complexes and p-type behavior of the photocathode. The results presented here show that the polymer backbone behaves like classical molecularly sensitized NiO photocathodes and operates as a hole accepting semiconductor. This in turn demonstrates the feasibility of all-polymer photocathodes for application in solar energy conversion.Ruri A. WahyuonoBianca SeidlerSebastian BoldAndrea DellithJan DellithJohannes AhnerPascal WintergerstGrace LoweMartin D. HagerMaria WächtlerCarsten StrebUlrich S. SchubertSven RauBenjamin DietzekNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-13 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Ruri A. Wahyuono Bianca Seidler Sebastian Bold Andrea Dellith Jan Dellith Johannes Ahner Pascal Wintergerst Grace Lowe Martin D. Hager Maria Wächtler Carsten Streb Ulrich S. Schubert Sven Rau Benjamin Dietzek Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
description	Abstract A conductive polymer (poly(p-phenylenevinylene), PPV) was covalently modified with RuII complexes to develop an all-polymer photocathode as a conceptual alternative to dye-sensitized NiO, which is the current state-of-the-art photocathode in solar fuels research. Photocathodes require efficient light-induced charge-transfer processes and we investigated these processes within our photocathodes using spectroscopic and spectro-electrochemical techniques. Ultrafast hole-injection dynamics in the polymer were investigated by transient absorption spectroscopy and charge transfer at the electrode–electrolyte interface was examined with chopped-light chronoamperometry. Light-induced hole injection from the photosensitizers into the PPV backbone was observed within 10 ps and the resulting charge-separated state (CSS) recombined within ~ 5 ns. This is comparable to CSS lifetimes of conventional NiO-photocathodes. Chopped-light chronoamperometry indicates enhanced charge-transfer at the electrode–electrolyte interface upon sensitization of the PPV with the RuII complexes and p-type behavior of the photocathode. The results presented here show that the polymer backbone behaves like classical molecularly sensitized NiO photocathodes and operates as a hole accepting semiconductor. This in turn demonstrates the feasibility of all-polymer photocathodes for application in solar energy conversion.
format	article
author	Ruri A. Wahyuono Bianca Seidler Sebastian Bold Andrea Dellith Jan Dellith Johannes Ahner Pascal Wintergerst Grace Lowe Martin D. Hager Maria Wächtler Carsten Streb Ulrich S. Schubert Sven Rau Benjamin Dietzek
author_facet	Ruri A. Wahyuono Bianca Seidler Sebastian Bold Andrea Dellith Jan Dellith Johannes Ahner Pascal Wintergerst Grace Lowe Martin D. Hager Maria Wächtler Carsten Streb Ulrich S. Schubert Sven Rau Benjamin Dietzek
author_sort	Ruri A. Wahyuono
title	Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
title_short	Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
title_full	Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
title_fullStr	Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
title_full_unstemmed	Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
title_sort	photocathodes beyond nio: charge transfer dynamics in a π-conjugated polymer functionalized with ru photosensitizers
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/9a04f15eb5e3486d934ccb2afd9c3d19
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Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers

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