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Low-Temperature Water–Gas Shift: Doping Ceria Improves Reducibility and Mobility of O-Bound Species and Catalyst Activity

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Abstract

A series of platinum loaded catalysts supported on cation (Me)-doped cerium dioxide (Me = Ba, La, Y, Hf and Zn) was prepared by co-precipitation of the Me-nitrates and impregnation of a Pt precursor. Low temperature water–gas shift activity depends on the nature of dopant employed, varying in the order of Ba > Y > Hf > La > undoped ceria > Zn. TPR-XANES measurements with flowing hydrogen reveal that adding dopants to ceria facilitate ceria reduction and increases the extents of both surface shell and bulk reduction of ceria. Experimental results confirm past theoretical models that dopants enhance both O-mobility and reducibility of ceria. DRIFTS measurements of the transient decomposition of formates in steam suggest that formate half-life follows the trend Zn > undoped ceria > La > Hf > Y > Ba, indicating that the formate decomposition rate is enhanced by the addition of most of the dopants tested. Taken together, the results suggest that dopant addition improves the WGS rate by increasing the O-mobility of O-bound associated intermediates. Therefore, less Pt and Ce, which are expensive, is required to achieve comparable levels of activity.

Graphical Abstract

TPR-XANES profiles of 0.5% Pt/ceria catalyst with and without Y-dopant.

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Acknowledgments

The work carried out at the CAER was supported in part by funding from the Commonwealth of Kentucky. Argonne’s research was supported in part by the U.S. Department of Energy (DOE), Office of Fossil Energy, National Energy Technology Laboratory (NETL). The use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions.

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Authors and Affiliations

  1. University of Kentucky Center for Applied Energy Research, 2540 Research Park Drive, Lexington, KY, 40511, USA

    Linda Z. Linganiso, Venkat Ramana Rao Pendyala, Gary Jacobs & Burtron H. Davis

  2. Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, CSE/205, Argonne, IL, 60439-4837, USA

    Donald C. Cronauer, A. Jeremy Kropf & Christopher L. Marshall

Authors
  1. Linda Z. Linganiso
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  2. Venkat Ramana Rao Pendyala
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  3. Gary Jacobs
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  4. Burtron H. Davis
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  5. Donald C. Cronauer
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  6. A. Jeremy Kropf
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  7. Christopher L. Marshall
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Correspondence to Burtron H. Davis.

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Linganiso, L.Z., Pendyala, V.R.R., Jacobs, G. et al. Low-Temperature Water–Gas Shift: Doping Ceria Improves Reducibility and Mobility of O-Bound Species and Catalyst Activity. Catal Lett 141, 1723–1731 (2011). https://doi.org/10.1007/s10562-011-0720-1

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  • DOI: https://doi.org/10.1007/s10562-011-0720-1

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