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Title: Factors Influencing the Stability of Au-Incorporated Metal-Oxide Supported Thin Films for Optical Gas Sensing

Abstract

There is interest in using Au-nanoparticle incorporated oxide films as functional sensor layers for high-temperature applications in optical-based sensors for measurements in both highly-oxidizing and highly-reducing atmospheres at temperatures approaching 900°C-1000°C because of a relatively high melting temperature combined with the inert nature of Au nanoparticles. This study includes a systematic series of experiments and theoretical calculations targeted at further understanding stability of Au-nanoparticle incorporated TiO2 films as archetype sensing materials. A combination of thermodynamic modeling and long-term exposure tests were utilized to unambiguously determine that gas stream composition-dependent reactive evaporation of Au (to form predominately Au(g) or AuH(g), depending upon the environment) at the surface of the nanoparticles is the dominant mechanism for mass loss of Au. Primary factors dictating the rate of reactive evaporation, and hence the associated film stability, were determined to be the gas stream temperature and the concentration of H2, with the former playing a more significant role over the ranges of temperatures (700°C - 800°C) and H2 concentrations (1% to 29% H2 by volume) explored. The mitigation of Au-mass loss through reactive evaporation was also successfully demonstrated by depositing a SiO2 overlayer on the Au-nanoparticle embedded films to prevent direct Au-nanoparticle/vapor-phase contact.

Authors:
 [1];  [2];  [2];  [1]
  1. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  2. National Energy Technology Lab. (NETL), Albany, OR (United States)
Publication Date:
Research Org.:
National Energy Technology Laboratory, Pittsburgh, PA (United States). In-house Research; Albany Research Center (ARC), Albany, OR (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1374181
Report Number(s):
NETL-PUB-20904
Journal ID: ISSN 0013-4651
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 4; Conference: Meeting of the Society, Honolulu, HI (United States), 2-7 Oct 2016; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Thin Films; Optical Gas Sensing; Au Nanoparticle; Hydrogen; Fuel Gas; X-ray Photoelectron Spectroscopy

Citation Formats

Baltrus, John P., Holcomb, Gordon R., Tylczak, Joseph H., and Ohodnicki, Paul R. Factors Influencing the Stability of Au-Incorporated Metal-Oxide Supported Thin Films for Optical Gas Sensing. United States: N. p., 2017. Web. doi:10.1149/2.1451704jes.
Baltrus, John P., Holcomb, Gordon R., Tylczak, Joseph H., & Ohodnicki, Paul R. Factors Influencing the Stability of Au-Incorporated Metal-Oxide Supported Thin Films for Optical Gas Sensing. United States. https://doi.org/10.1149/2.1451704jes
Baltrus, John P., Holcomb, Gordon R., Tylczak, Joseph H., and Ohodnicki, Paul R. 2017. "Factors Influencing the Stability of Au-Incorporated Metal-Oxide Supported Thin Films for Optical Gas Sensing". United States. https://doi.org/10.1149/2.1451704jes. https://www.osti.gov/servlets/purl/1374181.
@article{osti_1374181,
title = {Factors Influencing the Stability of Au-Incorporated Metal-Oxide Supported Thin Films for Optical Gas Sensing},
author = {Baltrus, John P. and Holcomb, Gordon R. and Tylczak, Joseph H. and Ohodnicki, Paul R.},
abstractNote = {There is interest in using Au-nanoparticle incorporated oxide films as functional sensor layers for high-temperature applications in optical-based sensors for measurements in both highly-oxidizing and highly-reducing atmospheres at temperatures approaching 900°C-1000°C because of a relatively high melting temperature combined with the inert nature of Au nanoparticles. This study includes a systematic series of experiments and theoretical calculations targeted at further understanding stability of Au-nanoparticle incorporated TiO2 films as archetype sensing materials. A combination of thermodynamic modeling and long-term exposure tests were utilized to unambiguously determine that gas stream composition-dependent reactive evaporation of Au (to form predominately Au(g) or AuH(g), depending upon the environment) at the surface of the nanoparticles is the dominant mechanism for mass loss of Au. Primary factors dictating the rate of reactive evaporation, and hence the associated film stability, were determined to be the gas stream temperature and the concentration of H2, with the former playing a more significant role over the ranges of temperatures (700°C - 800°C) and H2 concentrations (1% to 29% H2 by volume) explored. The mitigation of Au-mass loss through reactive evaporation was also successfully demonstrated by depositing a SiO2 overlayer on the Au-nanoparticle embedded films to prevent direct Au-nanoparticle/vapor-phase contact.},
doi = {10.1149/2.1451704jes},
url = {https://www.osti.gov/biblio/1374181}, journal = {Journal of the Electrochemical Society},
issn = {0013-4651},
number = 4,
volume = 164,
place = {United States},
year = {Fri Feb 24 00:00:00 EST 2017},
month = {Fri Feb 24 00:00:00 EST 2017}
}

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