DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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:
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. Fri . "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},
journal = {Journal of the Electrochemical Society},
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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Selective Plasmonic Gas Sensing: H 2 , NO 2 , and CO Spectral Discrimination by a Single Au-CeO 2 Nanocomposite Film
journal, June 2012

  • Joy, Nicholas A.; Nandasiri, Manjula I.; Rogers, Phillip H.
  • Analytical Chemistry, Vol. 84, Issue 11
  • DOI: 10.1021/ac3006846

High-Temperature Ceramic Gas Sensors: A Review
journal, July 2006


Calculation of Reactive-evaporation Rates of Chromia
journal, February 2008


Thermally stable Pt/mesoporous silica core–shell nanocatalysts for high-temperature reactions
journal, November 2008

  • Joo, Sang Hoon; Park, Jeong Young; Tsung, Chia-Kuang
  • Nature Materials, Vol. 8, Issue 2
  • DOI: 10.1038/nmat2329

Water Vapor–Mediated Volatilization of High-Temperature Materials
journal, July 2013


High temperature fiber-optic evanescent wave hydrogen sensors using La-doped SrTiO3 for SOFC applications
journal, December 2015

  • Schultz, Andrew M.; Brown, Thomas D.; Buric, Michael P.
  • Sensors and Actuators B: Chemical, Vol. 221
  • DOI: 10.1016/j.snb.2015.07.046

Solubility of fractal nanoparticles
journal, January 2007


Plasmonic-based Detection of NO 2 in a Harsh Environment
journal, May 2008

  • Rogers, Phillip H.; Sirinakis, George; Carpenter, Michael A.
  • The Journal of Physical Chemistry C, Vol. 112, Issue 24
  • DOI: 10.1021/jp800524z

In-situ and ex-situ characterization of TiO 2 and Au nanoparticle incorporated TiO 2 thin films for optical gas sensing at extreme temperatures
journal, March 2012

  • Ohodnicki, Paul R.; Wang, Congjun; Natesakhawat, Sittichai
  • Journal of Applied Physics, Vol. 111, Issue 6
  • DOI: 10.1063/1.3695380

Atomic Screening Constants from SCF Functions. II. Atoms with 37 to 86 Electrons
journal, August 1967

  • Clementi, E.; Raimondi, D. L.; Reinhardt, W. P.
  • The Journal of Chemical Physics, Vol. 47, Issue 4
  • DOI: 10.1063/1.1712084

Core-Satellite Nanocomposite Catalysts Protected by a Porous Silica Shell: Controllable Reactivity, High Stability, and Magnetic Recyclability
journal, November 2008

  • Ge, Jianping; Zhang, Qiao; Zhang, Tierui
  • Angewandte Chemie International Edition, Vol. 47, Issue 46
  • DOI: 10.1002/anie.200803968

Thermal Energy Harvesting Plasmonic Based Chemical Sensors
journal, October 2014

  • Karker, Nicholas; Dharmalingam, Gnanaprakash; Carpenter, Michael A.
  • ACS Nano, Vol. 8, Issue 10
  • DOI: 10.1021/nn504870b

Oxidation/Vaporization Kinetics of Cr2O3
journal, February 1971


Interactions of water vapor with oxides at elevated temperatures
journal, February 2005

  • Jacobson, Nathan; Myers, Dwight; Opila, Elizabeth
  • Journal of Physics and Chemistry of Solids, Vol. 66, Issue 2-4
  • DOI: 10.1016/j.jpcs.2004.06.044

Thermal stability and catalytic activity of gold nanoparticles supported on silica
journal, February 2009


High temperature optical sensing of gas and temperature using Au-nanoparticle incorporated oxides
journal, October 2014

  • Ohodnicki Jr., Paul R.; Brown, Thomas D.; Holcomb, Gordon R.
  • Sensors and Actuators B: Chemical, Vol. 202
  • DOI: 10.1016/j.snb.2014.04.106

High-Temperature-Stable Catalysts by Hollow Sphere Encapsulation
journal, December 2006

  • Arnal, Pablo M.; Comotti, Massimiliano; Schüth, Ferdi
  • Angewandte Chemie International Edition, Vol. 45, Issue 48
  • DOI: 10.1002/anie.200603507

New Method for Prediction of Binary Gas-Phase Diffusion Coefficients
journal, May 1966

  • Fuller, Edward N.; Schettler, Paul D.; Giddings, J. Calvin.
  • Industrial & Engineering Chemistry, Vol. 58, Issue 5
  • DOI: 10.1021/ie50677a007

Gold Nanoparticle-Doped TiO 2 Semiconductor Thin Films: Gas Sensing Properties
journal, December 2008

  • Buso, Dario; Post, Michael; Cantalini, Carlo
  • Advanced Functional Materials, Vol. 18, Issue 23
  • DOI: 10.1002/adfm.200800864

Thermochemistry of gaseous SiO(OH), SiO(OH) 2 , and SiO 2
journal, October 1994

  • Hildenbrand, D. L.; Lau, K. H.
  • The Journal of Chemical Physics, Vol. 101, Issue 7
  • DOI: 10.1063/1.467322

Three-dimensional thermo-fluid electrochemical modeling of planar SOFC stacks
journal, January 2003


Steam Oxidation and Chromia Evaporation in Ultrasupercritical Steam Boilers and Turbines
journal, January 2009

  • Holcomb, Gordon R.
  • Journal of The Electrochemical Society, Vol. 156, Issue 9
  • DOI: 10.1149/1.3155442

Principles of operation
book, January 1995


A Viscosity Equation for Gas Mixtures
journal, April 1950

  • Wilke, C. R.
  • The Journal of Chemical Physics, Vol. 18, Issue 4
  • DOI: 10.1063/1.1747673

SiC Recession Caused by SiO 2 Scale Volatility under Combustion Conditions: II, Thermodynamics and Gaseous-Diffusion Model
journal, July 1999


SiC Recession Caused by SiO 2 Scale Volatility under Combustion Conditions: I, Experimental Results and Empirical Model
journal, July 1999


Works referencing / citing this record:

Hydrogen transport during steam oxidation of iron and nickel alloys
journal, March 2019