A Silicon-Based Heterojunction Integrated with a Molecular Excited State in a Water-Splitting Tandem Cell

Bing Shan, M. Kyle Brennaman, Ludovic Troian-Gautier, Yanming Liu, Animesh Nayak, Christina M. Klug, Ting Ting Li, R Morris Bullock, Thomas J. Meyer

Research output: Contribution to journalArticle

Abstract

Semiconductor-based photocathodes with high light-absorption capability are of interest in the production of solar fuels, but many of them are limited by low efficiencies due to rapid interfacial back electron transfer. We demonstrate here that a nanowire-structured p-type Si (p-Si) electrode, surface-modified with a perylene-diimide derivative (PDI′), can undergo photoreduction of a surface-bound, water reduction catalyst toward efficient H2 evolution under a low applied bias. At the electrode interface, the PDI′ layer converts green light into high-energy holes at its excited state for extraction of photogenerated electrons at the photoexcited p-Si. The photogenerated electrons at the reduced PDI′ are subsequently transferred to the molecular H2-evolution catalyst. Involvement of the photoexcited PDI′ enables effective redox separation between the electrons at the reduced catalyst and the holes at the valence band of p-Si. The heterojunction photocathode was used in a tandem cell by coupling with a dye-sensitized photoanode for solar-driven water splitting into H2 and O2.

Original languageEnglish
JournalJournal of the American Chemical Society
DOIs
Publication statusPublished - Jan 1 2019

Fingerprint

Perylene
Silicon
Excited states
Heterojunctions
Electrons
Derivatives
Photocathodes
Water
Catalysts
Electrodes
Nanowires
Methyl Green
Semiconductors
Molecular Evolution
Valence bands
Light absorption
Oxidation-Reduction
Coloring Agents
Dyes
Semiconductor materials

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

A Silicon-Based Heterojunction Integrated with a Molecular Excited State in a Water-Splitting Tandem Cell. / Shan, Bing; Brennaman, M. Kyle; Troian-Gautier, Ludovic; Liu, Yanming; Nayak, Animesh; Klug, Christina M.; Li, Ting Ting; Bullock, R Morris; Meyer, Thomas J.

In: Journal of the American Chemical Society, 01.01.2019.

Research output: Contribution to journalArticle

Shan, Bing ; Brennaman, M. Kyle ; Troian-Gautier, Ludovic ; Liu, Yanming ; Nayak, Animesh ; Klug, Christina M. ; Li, Ting Ting ; Bullock, R Morris ; Meyer, Thomas J. / A Silicon-Based Heterojunction Integrated with a Molecular Excited State in a Water-Splitting Tandem Cell. In: Journal of the American Chemical Society. 2019.
@article{700efe76531846dc842edc3a82af6062,
title = "A Silicon-Based Heterojunction Integrated with a Molecular Excited State in a Water-Splitting Tandem Cell",
abstract = "Semiconductor-based photocathodes with high light-absorption capability are of interest in the production of solar fuels, but many of them are limited by low efficiencies due to rapid interfacial back electron transfer. We demonstrate here that a nanowire-structured p-type Si (p-Si) electrode, surface-modified with a perylene-diimide derivative (PDI′), can undergo photoreduction of a surface-bound, water reduction catalyst toward efficient H2 evolution under a low applied bias. At the electrode interface, the PDI′ layer converts green light into high-energy holes at its excited state for extraction of photogenerated electrons at the photoexcited p-Si. The photogenerated electrons at the reduced PDI′ are subsequently transferred to the molecular H2-evolution catalyst. Involvement of the photoexcited PDI′ enables effective redox separation between the electrons at the reduced catalyst and the holes at the valence band of p-Si. The heterojunction photocathode was used in a tandem cell by coupling with a dye-sensitized photoanode for solar-driven water splitting into H2 and O2.",
author = "Bing Shan and Brennaman, {M. Kyle} and Ludovic Troian-Gautier and Yanming Liu and Animesh Nayak and Klug, {Christina M.} and Li, {Ting Ting} and Bullock, {R Morris} and Meyer, {Thomas J.}",
year = "2019",
month = "1",
day = "1",
doi = "10.1021/jacs.9b04238",
language = "English",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "American Chemical Society",

}

TY - JOUR

T1 - A Silicon-Based Heterojunction Integrated with a Molecular Excited State in a Water-Splitting Tandem Cell

AU - Shan, Bing

AU - Brennaman, M. Kyle

AU - Troian-Gautier, Ludovic

AU - Liu, Yanming

AU - Nayak, Animesh

AU - Klug, Christina M.

AU - Li, Ting Ting

AU - Bullock, R Morris

AU - Meyer, Thomas J.

PY - 2019/1/1

Y1 - 2019/1/1

N2 - Semiconductor-based photocathodes with high light-absorption capability are of interest in the production of solar fuels, but many of them are limited by low efficiencies due to rapid interfacial back electron transfer. We demonstrate here that a nanowire-structured p-type Si (p-Si) electrode, surface-modified with a perylene-diimide derivative (PDI′), can undergo photoreduction of a surface-bound, water reduction catalyst toward efficient H2 evolution under a low applied bias. At the electrode interface, the PDI′ layer converts green light into high-energy holes at its excited state for extraction of photogenerated electrons at the photoexcited p-Si. The photogenerated electrons at the reduced PDI′ are subsequently transferred to the molecular H2-evolution catalyst. Involvement of the photoexcited PDI′ enables effective redox separation between the electrons at the reduced catalyst and the holes at the valence band of p-Si. The heterojunction photocathode was used in a tandem cell by coupling with a dye-sensitized photoanode for solar-driven water splitting into H2 and O2.

AB - Semiconductor-based photocathodes with high light-absorption capability are of interest in the production of solar fuels, but many of them are limited by low efficiencies due to rapid interfacial back electron transfer. We demonstrate here that a nanowire-structured p-type Si (p-Si) electrode, surface-modified with a perylene-diimide derivative (PDI′), can undergo photoreduction of a surface-bound, water reduction catalyst toward efficient H2 evolution under a low applied bias. At the electrode interface, the PDI′ layer converts green light into high-energy holes at its excited state for extraction of photogenerated electrons at the photoexcited p-Si. The photogenerated electrons at the reduced PDI′ are subsequently transferred to the molecular H2-evolution catalyst. Involvement of the photoexcited PDI′ enables effective redox separation between the electrons at the reduced catalyst and the holes at the valence band of p-Si. The heterojunction photocathode was used in a tandem cell by coupling with a dye-sensitized photoanode for solar-driven water splitting into H2 and O2.

UR - http://www.scopus.com/inward/record.url?scp=85068309827&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85068309827&partnerID=8YFLogxK

U2 - 10.1021/jacs.9b04238

DO - 10.1021/jacs.9b04238

M3 - Article

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

ER -