Pulsed-reactant in situ studies of ceria/CuO catalysts using simultaneous XRD, PDF and DRIFTS measurements

J. C. Hanson; R. Si; W. Xu; S. D. Senanayake; K. Mudiyanselage; D. Stacchiola; J. A. Rodriguez; H. Zhao; K. A. Beyer; G. Jennings; K. W. Chapman; P. J. Chupas; A. Martínez-Arias

doi:10.1016/j.cattod.2013.10.087

Pulsed-reactant in situ studies of ceria/CuO catalysts using simultaneous XRD, PDF and DRIFTS measurements

J. C. Hanson
, R. Si
, W. Xu
, S. D. Senanayake
, K. Mudiyanselage
, D. Stacchiola
, J. A. Rodriguez
, H. Zhao
, K. A. Beyer
, G. Jennings
, K. W. Chapman
, P. J. Chupas
, A. Martínez-Arias

Chemistry

Brookhaven National Laboratory
United States Department of Energy
CSIC - Instituto de Catálisis y Petroleoquímica (ICP)

Research output: Contribution to journal › Article › peer-review

29 Scopus citations

Abstract

The transient reduction-oxidation (redox) response of a ceria/CuO catalyst has been studied with pulsed gas techniques. The experimental setup allowed for simultaneous measurement of X-ray diffraction (XRD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) coupled to mass spectrometric (MS) analysis of reactants and products. The DRIFTS showed the bonding of CO to Cu_xO and formation of carbonates on ceria. The CO stretch signal was observed in the DRIFTS as the Cu₂O phase appeared in the simultaneous XRD pattern. This signal was still observed when XRD indicated that the Cu ₂O phase had converted to Cu(0). This unexpected result could arise from an amorphous surface of Cu₂O which could not be detected by XRD or because the surface sensitivity of the DRIFTS technique is much higher than the surface sensitivity of the XRD technique. Time-resolved pair distribution function (PDF) analysis was useful for tracking the appearance or disappearance of key structural features (CuO, CeO, CeCe, and CuCu) during the pulse experiments. The in situ PDF analysis provided new evidence that oxygen vacancies in the ceria could be detected with XRD data.

Original language	English
Pages (from-to)	64-71
Number of pages	8
Journal	Catalysis Today
Volume	229
DOIs	https://doi.org/10.1016/j.cattod.2013.10.087
State	Published - Jun 15 2014

Keywords

Catalyst
Combined DRIFTS/XRD
Cu/ceria
In situ XRD
Pair distribution function

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10.1016/j.cattod.2013.10.087

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Hanson, J. C., Si, R., Xu, W., Senanayake, S. D., Mudiyanselage, K., Stacchiola, D., Rodriguez, J. A., Zhao, H., Beyer, K. A., Jennings, G., Chapman, K. W., Chupas, P. J., & Martínez-Arias, A. (2014). Pulsed-reactant in situ studies of ceria/CuO catalysts using simultaneous XRD, PDF and DRIFTS measurements. Catalysis Today, 229, 64-71. https://doi.org/10.1016/j.cattod.2013.10.087

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title = "Pulsed-reactant in situ studies of ceria/CuO catalysts using simultaneous XRD, PDF and DRIFTS measurements",

abstract = "The transient reduction-oxidation (redox) response of a ceria/CuO catalyst has been studied with pulsed gas techniques. The experimental setup allowed for simultaneous measurement of X-ray diffraction (XRD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) coupled to mass spectrometric (MS) analysis of reactants and products. The DRIFTS showed the bonding of CO to CuxO and formation of carbonates on ceria. The CO stretch signal was observed in the DRIFTS as the Cu2O phase appeared in the simultaneous XRD pattern. This signal was still observed when XRD indicated that the Cu 2O phase had converted to Cu(0). This unexpected result could arise from an amorphous surface of Cu2O which could not be detected by XRD or because the surface sensitivity of the DRIFTS technique is much higher than the surface sensitivity of the XRD technique. Time-resolved pair distribution function (PDF) analysis was useful for tracking the appearance or disappearance of key structural features (CuO, CeO, CeCe, and CuCu) during the pulse experiments. The in situ PDF analysis provided new evidence that oxygen vacancies in the ceria could be detected with XRD data.",

keywords = "Catalyst, Combined DRIFTS/XRD, Cu/ceria, In situ XRD, Pair distribution function",

author = "Hanson, \{J. C.\} and R. Si and W. Xu and Senanayake, \{S. D.\} and K. Mudiyanselage and D. Stacchiola and Rodriguez, \{J. A.\} and H. Zhao and Beyer, \{K. A.\} and G. Jennings and Chapman, \{K. W.\} and Chupas, \{P. J.\} and A. Mart{\'i}nez-Arias",

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doi = "10.1016/j.cattod.2013.10.087",

language = "English",

volume = "229",

pages = "64--71",

journal = "Catalysis Today",

issn = "0920-5861",

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T1 - Pulsed-reactant in situ studies of ceria/CuO catalysts using simultaneous XRD, PDF and DRIFTS measurements

AU - Hanson, J. C.

AU - Si, R.

AU - Xu, W.

AU - Senanayake, S. D.

AU - Mudiyanselage, K.

AU - Stacchiola, D.

AU - Rodriguez, J. A.

AU - Zhao, H.

AU - Beyer, K. A.

AU - Jennings, G.

AU - Chapman, K. W.

AU - Chupas, P. J.

AU - Martínez-Arias, A.

PY - 2014/6/15

Y1 - 2014/6/15

N2 - The transient reduction-oxidation (redox) response of a ceria/CuO catalyst has been studied with pulsed gas techniques. The experimental setup allowed for simultaneous measurement of X-ray diffraction (XRD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) coupled to mass spectrometric (MS) analysis of reactants and products. The DRIFTS showed the bonding of CO to CuxO and formation of carbonates on ceria. The CO stretch signal was observed in the DRIFTS as the Cu2O phase appeared in the simultaneous XRD pattern. This signal was still observed when XRD indicated that the Cu 2O phase had converted to Cu(0). This unexpected result could arise from an amorphous surface of Cu2O which could not be detected by XRD or because the surface sensitivity of the DRIFTS technique is much higher than the surface sensitivity of the XRD technique. Time-resolved pair distribution function (PDF) analysis was useful for tracking the appearance or disappearance of key structural features (CuO, CeO, CeCe, and CuCu) during the pulse experiments. The in situ PDF analysis provided new evidence that oxygen vacancies in the ceria could be detected with XRD data.

AB - The transient reduction-oxidation (redox) response of a ceria/CuO catalyst has been studied with pulsed gas techniques. The experimental setup allowed for simultaneous measurement of X-ray diffraction (XRD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) coupled to mass spectrometric (MS) analysis of reactants and products. The DRIFTS showed the bonding of CO to CuxO and formation of carbonates on ceria. The CO stretch signal was observed in the DRIFTS as the Cu2O phase appeared in the simultaneous XRD pattern. This signal was still observed when XRD indicated that the Cu 2O phase had converted to Cu(0). This unexpected result could arise from an amorphous surface of Cu2O which could not be detected by XRD or because the surface sensitivity of the DRIFTS technique is much higher than the surface sensitivity of the XRD technique. Time-resolved pair distribution function (PDF) analysis was useful for tracking the appearance or disappearance of key structural features (CuO, CeO, CeCe, and CuCu) during the pulse experiments. The in situ PDF analysis provided new evidence that oxygen vacancies in the ceria could be detected with XRD data.

KW - Catalyst

KW - Combined DRIFTS/XRD

KW - Cu/ceria

KW - In situ XRD

KW - Pair distribution function

UR - https://www.scopus.com/pages/publications/84897092735

U2 - 10.1016/j.cattod.2013.10.087

DO - 10.1016/j.cattod.2013.10.087

M3 - Article

AN - SCOPUS:84897092735

SN - 0920-5861

VL - 229

SP - 64

EP - 71

JO - Catalysis Today

JF - Catalysis Today

ER -

Pulsed-reactant in situ studies of ceria/CuO catalysts using simultaneous XRD, PDF and DRIFTS measurements

Abstract

Keywords

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