Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients

The electrodeposition of noble metals, particularly gold, on semiconducting surfaces is a common step in the development of optoelectronic and catalytic devices. Theoretical models of electrodeposition transients can provide mechanistic insights on nucleation and growth of metal particles. Here we s...

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Main Authors: Vogel, Yan, Darwish, Nadim, Kashi, M., Gooding, J., Ciampi, Simone
Format: Journal Article
Published: Pergamon 2017
Online Access:http://purl.org/au-research/grants/arc/DE160100732
http://hdl.handle.net/20.500.11937/55697
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author Vogel, Yan
Darwish, Nadim
Kashi, M.
Gooding, J.
Ciampi, Simone
author_facet Vogel, Yan
Darwish, Nadim
Kashi, M.
Gooding, J.
Ciampi, Simone
author_sort Vogel, Yan
building Curtin Institutional Repository
collection Online Access
description The electrodeposition of noble metals, particularly gold, on semiconducting surfaces is a common step in the development of optoelectronic and catalytic devices. Theoretical models of electrodeposition transients can provide mechanistic insights on nucleation and growth of metal particles. Here we study to what extent these models can be applied to the growth of gold nanoparticles on semiconductor photoelectrodes, with the ultimate purpose of being able to control in two dimensions the electrodepostion process. We have examined current transients for the reduction of aurate salts at Si(100) photocathodes and have made adjustments both to the experimental parameters as well as to the available models so as to account for parallel adsorption steps. We have observed to what extent these models hold predictive power for a nucleation process on semiconducting photoelectrodes. We found that the hydrogen evolution reaction is significant even at very basic pH values, leading to a poor match between the modelled and actual outcomes in electrodeposition experiments. We have concluded that the catalytic activity of gold particles and semiconductor photoeffects make it difficult to rely on current transients alone to refine the experimental conditions for the growth of gold particles on Si(100) photocathodes. Specifically, it is proposed that hydrogen evolution causes turbulence leading to the displacement of particles and significant aggregation on the surface. A solution to this problem is to electrodeposit metals with high overpotentials for hydrogen evolution, such as copper, which allows us to control nucleation and ultimately to use illumination patterns to spatially address nanoparticle deposition on semiconducting surfaces.
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spelling curtin-20.500.11937-556972022-09-07T01:54:23Z Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients Vogel, Yan Darwish, Nadim Kashi, M. Gooding, J. Ciampi, Simone The electrodeposition of noble metals, particularly gold, on semiconducting surfaces is a common step in the development of optoelectronic and catalytic devices. Theoretical models of electrodeposition transients can provide mechanistic insights on nucleation and growth of metal particles. Here we study to what extent these models can be applied to the growth of gold nanoparticles on semiconductor photoelectrodes, with the ultimate purpose of being able to control in two dimensions the electrodepostion process. We have examined current transients for the reduction of aurate salts at Si(100) photocathodes and have made adjustments both to the experimental parameters as well as to the available models so as to account for parallel adsorption steps. We have observed to what extent these models hold predictive power for a nucleation process on semiconducting photoelectrodes. We found that the hydrogen evolution reaction is significant even at very basic pH values, leading to a poor match between the modelled and actual outcomes in electrodeposition experiments. We have concluded that the catalytic activity of gold particles and semiconductor photoeffects make it difficult to rely on current transients alone to refine the experimental conditions for the growth of gold particles on Si(100) photocathodes. Specifically, it is proposed that hydrogen evolution causes turbulence leading to the displacement of particles and significant aggregation on the surface. A solution to this problem is to electrodeposit metals with high overpotentials for hydrogen evolution, such as copper, which allows us to control nucleation and ultimately to use illumination patterns to spatially address nanoparticle deposition on semiconducting surfaces. 2017 Journal Article http://hdl.handle.net/20.500.11937/55697 10.1016/j.electacta.2017.06.126 http://purl.org/au-research/grants/arc/DE160100732 http://purl.org/au-research/grants/arc/DE160101101 Pergamon restricted
spellingShingle Vogel, Yan
Darwish, Nadim
Kashi, M.
Gooding, J.
Ciampi, Simone
Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients
title Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients
title_full Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients
title_fullStr Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients
title_full_unstemmed Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients
title_short Hydrogen evolution during the electrodeposition of gold nanoparticles at Si(100) photoelectrodes impairs the analysis of current-time transients
title_sort hydrogen evolution during the electrodeposition of gold nanoparticles at si(100) photoelectrodes impairs the analysis of current-time transients
url http://purl.org/au-research/grants/arc/DE160100732
http://purl.org/au-research/grants/arc/DE160100732
http://hdl.handle.net/20.500.11937/55697