Unraveling the dynamic nature of a CuO/CeO2 catalyst for CO oxidation in Operando: A combined study of XANES (fluorescence) and drifts

Siyu Yao; Kumudu Mudiyanselage; Wenqian Xu; Aaron C. Johnston-Peck; Jonathan C. Hanson; Tianpin Wu; Dario Stacchiola; José A. Rodriguez; Haiyan Zhao; Kevin A. Beyer; Karena W. Chapman; Peter J. Chupas; Arturo Martínez-Arias; Rui Si; Trudy B. Bolin; Wenjian Liu; Sanjaya D. Senanayake

doi:10.1021/cs500148e

Unraveling the dynamic nature of a CuO/CeO₂ catalyst for CO oxidation in Operando: A combined study of XANES (fluorescence) and drifts

Siyu Yao
, Kumudu Mudiyanselage
, Wenqian Xu
, Aaron C. Johnston-Peck
, Jonathan C. Hanson
, Tianpin Wu
, Dario Stacchiola
, José A. Rodriguez
, Haiyan Zhao
, Kevin A. Beyer
, Karena W. Chapman
, Peter J. Chupas
, Arturo Martínez-Arias
, Rui Si
, Trudy B. Bolin
, Wenjian Liu
, Sanjaya D. Senanayake

Chemistry

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

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

146 Scopus citations

Abstract

The redox chemistry and CO oxidation (2CO + O₂ → 2CO ₂) activity of catalysts generated by the dispersion of CuO on CeO₂ nanorods were investigated using a multitechnique approach. Combined measurements of time-resolved X-ray absorption near-edge spectroscopy (XANES) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in one setup were made possible with the development of a novel reaction cell in which fluorescence mode detection was applied to collect the XANES spectra. This is the first reported example using XANES in a similar technique combination. With the assistance of parallel time-resolved X-ray diffraction (XRD) measurements under operando conditions, we successfully probed the redox behavior of CuO/CeO₂ under CO reduction, constant-flow (steady-state) CO oxidation and during CO/O₂ cycling reactions. A strong copper ↔ ceria synergistic effect was observed in the CuO/CeO₂ catalyst. Surface Cu(I) species were found to exhibit a strong correlation with the catalyst activity for the CO oxidation reaction. By analysis of phase transformations as well as changes in oxidation state during the nonsteady states in the CO/O₂ cycling reaction, we collected information on the relative transformation rates of key species. Elementary steps in the mechanism for the CO oxidation reaction are proposed based on the understandings gained from the XANES/DRIFTS operando studies.

Original language	English
Pages (from-to)	1650-1661
Number of pages	12
Journal	ACS Catalysis
Volume	4
Issue number	6
DOIs	https://doi.org/10.1021/cs500148e
State	Published - Jun 6 2014

Keywords

ceria
CO oxidation
copper
DRIFTS
Operando catalysis
XANES

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10.1021/cs500148e

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Yao, S., Mudiyanselage, K., Xu, W., Johnston-Peck, A. C., Hanson, J. C., Wu, T., Stacchiola, D., Rodriguez, J. A., Zhao, H., Beyer, K. A., Chapman, K. W., Chupas, P. J., Martínez-Arias, A., Si, R., Bolin, T. B., Liu, W., & Senanayake, S. D. (2014). Unraveling the dynamic nature of a CuO/CeO₂ catalyst for CO oxidation in Operando: A combined study of XANES (fluorescence) and drifts. ACS Catalysis, 4(6), 1650-1661. https://doi.org/10.1021/cs500148e

@article{c7fa09541fc141c291f34475e4c215f7,

title = "Unraveling the dynamic nature of a CuO/CeO2 catalyst for CO oxidation in Operando: A combined study of XANES (fluorescence) and drifts",

abstract = "The redox chemistry and CO oxidation (2CO + O2 → 2CO 2) activity of catalysts generated by the dispersion of CuO on CeO2 nanorods were investigated using a multitechnique approach. Combined measurements of time-resolved X-ray absorption near-edge spectroscopy (XANES) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in one setup were made possible with the development of a novel reaction cell in which fluorescence mode detection was applied to collect the XANES spectra. This is the first reported example using XANES in a similar technique combination. With the assistance of parallel time-resolved X-ray diffraction (XRD) measurements under operando conditions, we successfully probed the redox behavior of CuO/CeO2 under CO reduction, constant-flow (steady-state) CO oxidation and during CO/O2 cycling reactions. A strong copper ↔ ceria synergistic effect was observed in the CuO/CeO2 catalyst. Surface Cu(I) species were found to exhibit a strong correlation with the catalyst activity for the CO oxidation reaction. By analysis of phase transformations as well as changes in oxidation state during the nonsteady states in the CO/O2 cycling reaction, we collected information on the relative transformation rates of key species. Elementary steps in the mechanism for the CO oxidation reaction are proposed based on the understandings gained from the XANES/DRIFTS operando studies.",

keywords = "ceria, CO oxidation, copper, DRIFTS, Operando catalysis, XANES",

author = "Siyu Yao and Kumudu Mudiyanselage and Wenqian Xu and Johnston-Peck, \{Aaron C.\} and Hanson, \{Jonathan C.\} and Tianpin Wu and Dario Stacchiola and Rodriguez, \{Jos{\'e} A.\} and Haiyan Zhao and Beyer, \{Kevin A.\} and Chapman, \{Karena W.\} and Chupas, \{Peter J.\} and Arturo Mart{\'i}nez-Arias and Rui Si and Bolin, \{Trudy B.\} and Wenjian Liu and Senanayake, \{Sanjaya D.\}",

year = "2014",

month = jun,

day = "6",

doi = "10.1021/cs500148e",

language = "English",

volume = "4",

pages = "1650--1661",

journal = "ACS Catalysis",

issn = "2155-5435",

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Yao, S, Mudiyanselage, K, Xu, W, Johnston-Peck, AC, Hanson, JC, Wu, T, Stacchiola, D, Rodriguez, JA, Zhao, H, Beyer, KA, Chapman, KW, Chupas, PJ, Martínez-Arias, A, Si, R, Bolin, TB, Liu, W & Senanayake, SD 2014, 'Unraveling the dynamic nature of a CuO/CeO₂ catalyst for CO oxidation in Operando: A combined study of XANES (fluorescence) and drifts', ACS Catalysis, vol. 4, no. 6, pp. 1650-1661. https://doi.org/10.1021/cs500148e

TY - JOUR

T1 - Unraveling the dynamic nature of a CuO/CeO2 catalyst for CO oxidation in Operando

T2 - A combined study of XANES (fluorescence) and drifts

AU - Yao, Siyu

AU - Mudiyanselage, Kumudu

AU - Xu, Wenqian

AU - Johnston-Peck, Aaron C.

AU - Hanson, Jonathan C.

AU - Wu, Tianpin

AU - Stacchiola, Dario

AU - Rodriguez, José A.

AU - Zhao, Haiyan

AU - Beyer, Kevin A.

AU - Chapman, Karena W.

AU - Chupas, Peter J.

AU - Martínez-Arias, Arturo

AU - Si, Rui

AU - Bolin, Trudy B.

AU - Liu, Wenjian

AU - Senanayake, Sanjaya D.

PY - 2014/6/6

Y1 - 2014/6/6

N2 - The redox chemistry and CO oxidation (2CO + O2 → 2CO 2) activity of catalysts generated by the dispersion of CuO on CeO2 nanorods were investigated using a multitechnique approach. Combined measurements of time-resolved X-ray absorption near-edge spectroscopy (XANES) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in one setup were made possible with the development of a novel reaction cell in which fluorescence mode detection was applied to collect the XANES spectra. This is the first reported example using XANES in a similar technique combination. With the assistance of parallel time-resolved X-ray diffraction (XRD) measurements under operando conditions, we successfully probed the redox behavior of CuO/CeO2 under CO reduction, constant-flow (steady-state) CO oxidation and during CO/O2 cycling reactions. A strong copper ↔ ceria synergistic effect was observed in the CuO/CeO2 catalyst. Surface Cu(I) species were found to exhibit a strong correlation with the catalyst activity for the CO oxidation reaction. By analysis of phase transformations as well as changes in oxidation state during the nonsteady states in the CO/O2 cycling reaction, we collected information on the relative transformation rates of key species. Elementary steps in the mechanism for the CO oxidation reaction are proposed based on the understandings gained from the XANES/DRIFTS operando studies.

AB - The redox chemistry and CO oxidation (2CO + O2 → 2CO 2) activity of catalysts generated by the dispersion of CuO on CeO2 nanorods were investigated using a multitechnique approach. Combined measurements of time-resolved X-ray absorption near-edge spectroscopy (XANES) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in one setup were made possible with the development of a novel reaction cell in which fluorescence mode detection was applied to collect the XANES spectra. This is the first reported example using XANES in a similar technique combination. With the assistance of parallel time-resolved X-ray diffraction (XRD) measurements under operando conditions, we successfully probed the redox behavior of CuO/CeO2 under CO reduction, constant-flow (steady-state) CO oxidation and during CO/O2 cycling reactions. A strong copper ↔ ceria synergistic effect was observed in the CuO/CeO2 catalyst. Surface Cu(I) species were found to exhibit a strong correlation with the catalyst activity for the CO oxidation reaction. By analysis of phase transformations as well as changes in oxidation state during the nonsteady states in the CO/O2 cycling reaction, we collected information on the relative transformation rates of key species. Elementary steps in the mechanism for the CO oxidation reaction are proposed based on the understandings gained from the XANES/DRIFTS operando studies.

KW - ceria

KW - CO oxidation

KW - copper

KW - DRIFTS

KW - Operando catalysis

KW - XANES

UR - https://www.scopus.com/pages/publications/84902160220

U2 - 10.1021/cs500148e

DO - 10.1021/cs500148e

M3 - Article

AN - SCOPUS:84902160220

SN - 2155-5435

VL - 4

SP - 1650

EP - 1661

JO - ACS Catalysis

JF - ACS Catalysis

IS - 6

ER -

Unraveling the dynamic nature of a CuO/CeO₂ catalyst for CO oxidation in Operando: A combined study of XANES (fluorescence) and drifts

Abstract

Keywords

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