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Title: Selective Plasmonic Gas Sensing: H2, NO2, and CO Spectral Discrimination by a Single Au-CeO2 Nanocomposite Film

Abstract

A Au-CeO2 nanocomposite film has been investigated as a potential sensing element for high-temperature plasmonic sensing of H2, CO, and NO2 in an oxygen containing environment. The CeO2 thin film was deposited by molecular beam epitaxy (MBE) and Au was implanted into the as-grown film at an elevated temperature followed by high temperature annealing to form well-defined Au nanoclusters. The Au-CeO2 nanocomposite film was characterized by x-ray diffraction (XRD) and Rutherford backscattering spectrometry (RBS). For the gas sensing experiments, separate exposures to varying concentrations of H2, CO, and NO2 were performed at a temperature of 500°C in oxygen backgrounds of 5.0, 10, and ~21% O2. Changes in the localized surface plasmon resonance (LSPR) absorption peak were monitored during gas exposures and are believed to be the result of oxidation-reduction processes that fill or create oxygen vacancies in the CeO2. This process affects the LSPR peak position either by charge exchange with the Au nanoparticles or by changes in the dielectric constant surrounding the particles. Multivariate analysis was used to gauge the inherent selectivity of the film between the separate analytes. From principal component analysis (PCA), unique and identifiable responses were seen for each of the analytes. Linear discriminant analysis (LDA)more » was also used and showed separation between analytes as well as trends in gas concentration. Results indicate that the Au-CeO2 thin film is selective to O2, H2, CO, and NO2 in separate exposures. Combined with the observed stability over long exposure periods, the Au-CeO2 film shows good potential as an optical sensing element for harsh environmental conditions.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1045097
Report Number(s):
PNNL-SA-85244
34895; KP1704020; TRN: US201214%%925
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Analytical Chemistry, 84(11):5025-5034
Additional Journal Information:
Journal Volume: 84; Journal Issue: 11
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ABSORPTION; ANNEALING; CHARGE EXCHANGE; MOLECULAR BEAM EPITAXY; MULTIVARIATE ANALYSIS; OXYGEN; PERMITTIVITY; PLASMONS; RESONANCE; RUTHERFORD BACKSCATTERING SPECTROSCOPY; STABILITY; THIN FILMS; VACANCIES; X-RAY DIFFRACTION; Selective; Plasmonic; Gas; Sensing; H2; NO2; and; CO; Discrimination; Single; Au-CeO2; Nanocomposite; Film; Environmental Molecular Sciences Laboratory

Citation Formats

Joy, N., Nandasiri, Manjula I., Rogers, Phillip H., Jiang, Weilin, Varga, Tamas, Kuchibhatla, Satyanarayana V N T, Thevuthasan, Suntharampillai, and Carpenter, Michael A. Selective Plasmonic Gas Sensing: H2, NO2, and CO Spectral Discrimination by a Single Au-CeO2 Nanocomposite Film. United States: N. p., 2012. Web. doi:10.1021/ac3006846.
Joy, N., Nandasiri, Manjula I., Rogers, Phillip H., Jiang, Weilin, Varga, Tamas, Kuchibhatla, Satyanarayana V N T, Thevuthasan, Suntharampillai, & Carpenter, Michael A. Selective Plasmonic Gas Sensing: H2, NO2, and CO Spectral Discrimination by a Single Au-CeO2 Nanocomposite Film. United States. doi:10.1021/ac3006846.
Joy, N., Nandasiri, Manjula I., Rogers, Phillip H., Jiang, Weilin, Varga, Tamas, Kuchibhatla, Satyanarayana V N T, Thevuthasan, Suntharampillai, and Carpenter, Michael A. Tue . "Selective Plasmonic Gas Sensing: H2, NO2, and CO Spectral Discrimination by a Single Au-CeO2 Nanocomposite Film". United States. doi:10.1021/ac3006846.
@article{osti_1045097,
title = {Selective Plasmonic Gas Sensing: H2, NO2, and CO Spectral Discrimination by a Single Au-CeO2 Nanocomposite Film},
author = {Joy, N. and Nandasiri, Manjula I. and Rogers, Phillip H. and Jiang, Weilin and Varga, Tamas and Kuchibhatla, Satyanarayana V N T and Thevuthasan, Suntharampillai and Carpenter, Michael A.},
abstractNote = {A Au-CeO2 nanocomposite film has been investigated as a potential sensing element for high-temperature plasmonic sensing of H2, CO, and NO2 in an oxygen containing environment. The CeO2 thin film was deposited by molecular beam epitaxy (MBE) and Au was implanted into the as-grown film at an elevated temperature followed by high temperature annealing to form well-defined Au nanoclusters. The Au-CeO2 nanocomposite film was characterized by x-ray diffraction (XRD) and Rutherford backscattering spectrometry (RBS). For the gas sensing experiments, separate exposures to varying concentrations of H2, CO, and NO2 were performed at a temperature of 500°C in oxygen backgrounds of 5.0, 10, and ~21% O2. Changes in the localized surface plasmon resonance (LSPR) absorption peak were monitored during gas exposures and are believed to be the result of oxidation-reduction processes that fill or create oxygen vacancies in the CeO2. This process affects the LSPR peak position either by charge exchange with the Au nanoparticles or by changes in the dielectric constant surrounding the particles. Multivariate analysis was used to gauge the inherent selectivity of the film between the separate analytes. From principal component analysis (PCA), unique and identifiable responses were seen for each of the analytes. Linear discriminant analysis (LDA) was also used and showed separation between analytes as well as trends in gas concentration. Results indicate that the Au-CeO2 thin film is selective to O2, H2, CO, and NO2 in separate exposures. Combined with the observed stability over long exposure periods, the Au-CeO2 film shows good potential as an optical sensing element for harsh environmental conditions.},
doi = {10.1021/ac3006846},
journal = {Analytical Chemistry, 84(11):5025-5034},
number = 11,
volume = 84,
place = {United States},
year = {2012},
month = {6}
}