1-(3'-Amino)propylsilatrane derivatives as covalent surface linkers to nanoparticulate metal oxide films for use in photoelectrochemical cells.

Bradley J. Brennan, Amy E. Keirstead, Paul A. Liddell, Sean A. Vail, Thomas A Moore, Ana L Moore, John Devens Gust

Research output: Contribution to journalArticle

40 Citations (Scopus)

Abstract

A triethanolamine-protected silane, 1-(3'-amino)propylsilatrane, was incorporated into the structure of porphyrin- and ruthenium-based dyes and used to link them to transparent semiconductor nanoparticulate metal oxide films. Silatrane reacts with the metal oxide to form strong, covalent silyl ether bonds. In this study, silatrane-functionalized dyes and analogous carboxylate-functionalized dyes were used as visible light sensitizers for porous nanoparticulate SnO(2) photoanodes. The performance of the dyes was compared in photoelectrochemical cells incorporating either non-regenerative or regenerative redox components. The non-regenerative cell used NADH (beta-nicotinamide adenine dinucleotide) as a sacrificial electron donor and Hg(2)SO(4)/Hg as a sacrificial cathode, whereas the regenerative cell used the iodide/triiodide redox couple. Experiments showed that the silyl ether bonding gave the electrodes increased stability toward sensitizer desorption compared to carboxylate surface linkages. Porphyrin-silatrane dyes also demonstrated similar or better performance than their carboxylate analogs in photoelectrochemical cells. The improvement correlates with the results from transient absorbance spectroscopy, which show that the longer linker on the silatrane porphyrins slows charge recombination between oxidized porphyrin and the electrode surface. The improved photoelectrochemical cell efficiency and stability of the silatrane-based dyes compared to carboxylates demonstrate that silatranes are promising agents for bonding organic molecules to metal oxide surfaces.

Original languageEnglish
Pages (from-to)505203
Number of pages1
JournalNanotechnology
Volume20
Issue number50
Publication statusPublished - Dec 16 2009

Fingerprint

Photoelectrochemical cells
Oxide films
Coloring Agents
Dyes
Metals
Porphyrins
Derivatives
NAD
Ether
Oxides
Ethers
Triethanolamine
Silanes
Electrodes
Ruthenium
Iodides
silatrane
Desorption
Cathodes
Spectroscopy

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Electrical and Electronic Engineering
  • Mechanical Engineering
  • Mechanics of Materials
  • Materials Science(all)

Cite this

1-(3'-Amino)propylsilatrane derivatives as covalent surface linkers to nanoparticulate metal oxide films for use in photoelectrochemical cells. / Brennan, Bradley J.; Keirstead, Amy E.; Liddell, Paul A.; Vail, Sean A.; Moore, Thomas A; Moore, Ana L; Gust, John Devens.

In: Nanotechnology, Vol. 20, No. 50, 16.12.2009, p. 505203.

Research output: Contribution to journalArticle

@article{12c4a80d25ce41d9ad8b33ce89dda263,
title = "1-(3'-Amino)propylsilatrane derivatives as covalent surface linkers to nanoparticulate metal oxide films for use in photoelectrochemical cells.",
abstract = "A triethanolamine-protected silane, 1-(3'-amino)propylsilatrane, was incorporated into the structure of porphyrin- and ruthenium-based dyes and used to link them to transparent semiconductor nanoparticulate metal oxide films. Silatrane reacts with the metal oxide to form strong, covalent silyl ether bonds. In this study, silatrane-functionalized dyes and analogous carboxylate-functionalized dyes were used as visible light sensitizers for porous nanoparticulate SnO(2) photoanodes. The performance of the dyes was compared in photoelectrochemical cells incorporating either non-regenerative or regenerative redox components. The non-regenerative cell used NADH (beta-nicotinamide adenine dinucleotide) as a sacrificial electron donor and Hg(2)SO(4)/Hg as a sacrificial cathode, whereas the regenerative cell used the iodide/triiodide redox couple. Experiments showed that the silyl ether bonding gave the electrodes increased stability toward sensitizer desorption compared to carboxylate surface linkages. Porphyrin-silatrane dyes also demonstrated similar or better performance than their carboxylate analogs in photoelectrochemical cells. The improvement correlates with the results from transient absorbance spectroscopy, which show that the longer linker on the silatrane porphyrins slows charge recombination between oxidized porphyrin and the electrode surface. The improved photoelectrochemical cell efficiency and stability of the silatrane-based dyes compared to carboxylates demonstrate that silatranes are promising agents for bonding organic molecules to metal oxide surfaces.",
author = "Brennan, {Bradley J.} and Keirstead, {Amy E.} and Liddell, {Paul A.} and Vail, {Sean A.} and Moore, {Thomas A} and Moore, {Ana L} and Gust, {John Devens}",
year = "2009",
month = "12",
day = "16",
language = "English",
volume = "20",
pages = "505203",
journal = "Nanotechnology",
issn = "0957-4484",
publisher = "IOP Publishing Ltd.",
number = "50",

}

TY - JOUR

T1 - 1-(3'-Amino)propylsilatrane derivatives as covalent surface linkers to nanoparticulate metal oxide films for use in photoelectrochemical cells.

AU - Brennan, Bradley J.

AU - Keirstead, Amy E.

AU - Liddell, Paul A.

AU - Vail, Sean A.

AU - Moore, Thomas A

AU - Moore, Ana L

AU - Gust, John Devens

PY - 2009/12/16

Y1 - 2009/12/16

N2 - A triethanolamine-protected silane, 1-(3'-amino)propylsilatrane, was incorporated into the structure of porphyrin- and ruthenium-based dyes and used to link them to transparent semiconductor nanoparticulate metal oxide films. Silatrane reacts with the metal oxide to form strong, covalent silyl ether bonds. In this study, silatrane-functionalized dyes and analogous carboxylate-functionalized dyes were used as visible light sensitizers for porous nanoparticulate SnO(2) photoanodes. The performance of the dyes was compared in photoelectrochemical cells incorporating either non-regenerative or regenerative redox components. The non-regenerative cell used NADH (beta-nicotinamide adenine dinucleotide) as a sacrificial electron donor and Hg(2)SO(4)/Hg as a sacrificial cathode, whereas the regenerative cell used the iodide/triiodide redox couple. Experiments showed that the silyl ether bonding gave the electrodes increased stability toward sensitizer desorption compared to carboxylate surface linkages. Porphyrin-silatrane dyes also demonstrated similar or better performance than their carboxylate analogs in photoelectrochemical cells. The improvement correlates with the results from transient absorbance spectroscopy, which show that the longer linker on the silatrane porphyrins slows charge recombination between oxidized porphyrin and the electrode surface. The improved photoelectrochemical cell efficiency and stability of the silatrane-based dyes compared to carboxylates demonstrate that silatranes are promising agents for bonding organic molecules to metal oxide surfaces.

AB - A triethanolamine-protected silane, 1-(3'-amino)propylsilatrane, was incorporated into the structure of porphyrin- and ruthenium-based dyes and used to link them to transparent semiconductor nanoparticulate metal oxide films. Silatrane reacts with the metal oxide to form strong, covalent silyl ether bonds. In this study, silatrane-functionalized dyes and analogous carboxylate-functionalized dyes were used as visible light sensitizers for porous nanoparticulate SnO(2) photoanodes. The performance of the dyes was compared in photoelectrochemical cells incorporating either non-regenerative or regenerative redox components. The non-regenerative cell used NADH (beta-nicotinamide adenine dinucleotide) as a sacrificial electron donor and Hg(2)SO(4)/Hg as a sacrificial cathode, whereas the regenerative cell used the iodide/triiodide redox couple. Experiments showed that the silyl ether bonding gave the electrodes increased stability toward sensitizer desorption compared to carboxylate surface linkages. Porphyrin-silatrane dyes also demonstrated similar or better performance than their carboxylate analogs in photoelectrochemical cells. The improvement correlates with the results from transient absorbance spectroscopy, which show that the longer linker on the silatrane porphyrins slows charge recombination between oxidized porphyrin and the electrode surface. The improved photoelectrochemical cell efficiency and stability of the silatrane-based dyes compared to carboxylates demonstrate that silatranes are promising agents for bonding organic molecules to metal oxide surfaces.

UR - http://www.scopus.com/inward/record.url?scp=77952487193&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=77952487193&partnerID=8YFLogxK

M3 - Article

C2 - 19923652

AN - SCOPUS:77952487193

VL - 20

SP - 505203

JO - Nanotechnology

JF - Nanotechnology

SN - 0957-4484

IS - 50

ER -