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

Publikationstyp:
Zeitschriftenaufsatz
Metadaten:
Autoren
  • Ruri A Wahyuono
  • Bianca Seidler
  • Sebastian Bold
  • Andrea Dellith
  • Jan Dellith
  • Johannes Ahner
  • Pascal Wintergerst
  • Grace Lowe
  • Martin D Hager
  • Maria Wachtler
  • Carsten Streb
  • Ulrich S Schubert
  • Sven Rau
  • Benjamin Dietzek
Autoren-URL
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000617706100024&DestLinkType=FullRecord&DestApp=WOS_CPL
DOI
10.1038/s41598-021-82395-x
Externe Identifier
  • Clarivate Analytics Document Solution ID: QG6PP
  • PubMed Identifier: 33531588
ISSN
2045-2322
Ausgabe der Veröffentlichung
1
Zeitschrift
SCIENTIFIC REPORTS
Artikelnummer
ARTN 2787
Datum der Veröffentlichung
2021
Status
Published
Titel
Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
Sub types
  • Article
Ausgabe der Zeitschrift
11

Datenquelle: Web of Science (Lite)

Andere Metadatenquellen:
Abstract
<jats:title>Abstract</jats:title><jats:p>A conductive polymer (poly(<jats:italic>p</jats:italic>-phenylenevinylene), <jats:bold>PPV</jats:bold>) was covalently modified with Ru<jats:sup>II</jats:sup> 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 Ru<jats:sup>II</jats:sup> 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.</jats:p>
Autoren
  • 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
DOI
10.1038/s41598-021-82395-x
eISSN
2045-2322
Ausgabe der Veröffentlichung
1
Zeitschrift
Scientific Reports
Sprache
en
Artikelnummer
2787
Online publication date
2021
Status
Published online
Herausgeber
Springer Science and Business Media LLC
Herausgeber URL
http://dx.doi.org/10.1038/s41598-021-82395-x
Datum der Datenerfassung
2022
Titel
Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers
Ausgabe der Zeitschrift
11

Datenquelle: Crossref

Abstract
A conductive polymer (poly(p-phenylenevinylene), PPV) was covalently modified with Ru<sup>II</sup> 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 Ru<sup>II</sup> 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.
Addresses
  • Department Functional Interfaces, Leibniz Institute of Photonic Technology (IPHT) Jena e.V., Albert-Einstein-Strasse 9, 07745, Jena, Germany.
Autoren
  • 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
DOI
10.1038/s41598-021-82395-x
eISSN
2045-2322
Externe Identifier
  • PubMed Identifier: 33531588
  • PubMed Central ID: PMC7854750
Funding acknowledgements
  • Deutsche Forschungsgemeinschaft: 364549901
  • Projekt DEAL:
  • Agence Nationale de la Recherche: ANR-15-IDEX-02
  • Deutscher Akademischer Austauschdienst:
Open access
true
ISSN
2045-2322
Ausgabe der Veröffentlichung
1
Zeitschrift
Scientific reports
Sprache
eng
Medium
Electronic
Online publication date
2021
Open access status
Open Access
Paginierung
2787
Datum der Veröffentlichung
2021
Status
Published
Publisher licence
CC BY
Datum der Datenerfassung
2021
Titel
Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers.
Sub types
  • research-article
  • Journal Article
Ausgabe der Zeitschrift
11

Files

https://www.nature.com/articles/s41598-021-82395-x.pdf https://europepmc.org/articles/PMC7854750?pdf=render

Datenquelle: Europe PubMed Central

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.
Date of acceptance
2021
Autoren
  • 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
Autoren-URL
https://www.ncbi.nlm.nih.gov/pubmed/33531588
DOI
10.1038/s41598-021-82395-x
eISSN
2045-2322
Externe Identifier
  • PubMed Central ID: PMC7854750
Funding acknowledgements
  • Agence Nationale de la Recherche: ANR-15-IDEX-02
  • Deutsche Forschungsgemeinschaft: 364549901
Ausgabe der Veröffentlichung
1
Zeitschrift
Sci Rep
Sprache
eng
Country
England
Paginierung
2787
PII
10.1038/s41598-021-82395-x
Datum der Veröffentlichung
2021
Status
Published online
Titel
Photocathodes beyond NiO: charge transfer dynamics in a π-conjugated polymer functionalized with Ru photosensitizers.
Sub types
  • Journal Article
Ausgabe der Zeitschrift
11

Datenquelle: PubMed

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