Advertisement

Emission Control Science and Technology

, Volume 5, Issue 4, pp 353–362 | Cite as

Three-way Catalysis with Noble Metal-Substituted La(Fe,Co)O3 Perovskites—the Role of Noble and Base Metal Components

  • Sascha Heikens
  • Viktor Ulrich
  • Pragati S. Joshi
  • Bilge Saruhan-Brings
  • Wolfgang GrünertEmail author
Special Issue: In Recognition of Professor Wolfgang Grünert's Contributions to the Science and Fundamentals of Selective Catalytic Reduction of NOx
First Online:
  • 57 Downloads

Abstract

La(FexCo1-x)O3 perovskites with noble metals incorporated (Pd in different amounts, Pt, Rh; with Pd at x ≈ 1, 0.7, 0) were prepared via the dry citrate method and examined with respect to their behavior in three-way catalysis (lean and stoichiometric model feeds containing CO, propene, NO, and O2) in the as-prepared state and after redox stress of different severity (at temperatures up 1173 K). Results were compared with data obtained with a commercial Pd-based three-way catalyst. Perovskites outperformed the reference in CO oxidation but were less active in propene oxidation and NO reduction. While their oxidation activity was rather stable, their NO reduction activity suffered severely from the redox treatments unlike that of the reference. It was concluded that oxidation and reduction reactions are catalyzed by different sites. While the presence and the nature of the noble metal were mostly irrelevant for oxidation reactions, in particular for CO oxidation, NO reduction was dominated by the contribution of the noble metal component. The inferior NO reduction activity despite noble metal contents of up to 2.5 wt% and the dominance of the perovskite surface in propene oxidation (compared with high oxidation activity of Pd in the reference catalyst) suggest that the metal component was not well exposed in the perovskite catalysts.

Keywords

TWC Perovskites Noble metals Activity Stability 
This is a preview of subscription content, log in to check access.

Notes

Acknowledgments

We thank Mrs. Susanne Buse and Dr. T. Reinicke for their support by physisorption experiments and XRD measurements.

Funding Information

We gratefully acknowledge financial support by the German Science Foundation (DFG, Grants No. Gr 1447/17 and SA 1343/5 within Priority Programme 1299).

Compliance with Ethical Standards

Conflict of Interest

The authors declare that they have no competing interests.

Supplementary material

40825_2019_123_MOESM1_ESM.docx (1.3 mb)
ESM 1 (DOCX 1.50 MB)

References

  1. 1.
    Mellor, J.R., Palazov, A.N., Grigorova, B.S., Greyling, J.F., Reddy, K., Letsoalo, M.P., Marsh, J.H.: The application of supported gold catalysts to automotive pollution abatement. Catal. Today. 72(1–2), 145–156 (2002)CrossRefGoogle Scholar
  2. 2.
    Ulrich, V., Moroz, B., Sinev, I., Pyriaev, P., Bukhtiyarov, V.I.: Studies on three-way catalysis with supported gold catalysts. Influence of support and water content in feed. Appl. Catal. B. 203, 572–581 (2017)CrossRefGoogle Scholar
  3. 3.
    Ulrich, V., Froese, C., Moroz, B., Pyrjaev, P., Gerasimov, E., Sinev, I., Roldan Cuenya, B., Muhler, M., Bukhtiyarov, V., Grünert, W.: Three-way catalysis with supported gold catalysts: poisoning effects of hydrocarbons. Appl. Catal. B. 237, 1021–1032 (2018)CrossRefGoogle Scholar
  4. 4.
    Nazarpoor, Z., Golden, S. J.: Zero-PGM catalyst with oxygen storage capacity for TWC systems. US Pat. 2015/0105245A1, published April 16, 2015, and a number of other US patents issued to CDTI Inc.Google Scholar
  5. 5.
    Glisenti, A., Pacella, M., Guiotto, M., Natile, M.M., Canu, P.: Largely Cu-doped LaCo1-xCuxO3 perovskites for TWC: toward new PGM-free catalysts. Appl. Catal. B. 180, 94–105 (2016)CrossRefGoogle Scholar
  6. 6.
    Schön, A., Dacquin, J.P., Dujardin, C., Granger, P.: Catalytic activity and thermal stability of LaFe1-xCuxO3 and La2CuO4 perovskite solids in three-way-catalysis. Top. Catal. 60(3–5), 300–306 (2017)CrossRefGoogle Scholar
  7. 7.
    Schön, A., Dujardin, C., Dacquin, J.P., Granger, P.: Enhancing catalytic activity of perovskite-based catalysts in three-way catalysis by surface composition optimisation. Catal. Today. 258(2), 543–548 (2016)Google Scholar
  8. 8.
    Zhou, C., Zhang, Y.X., Hu, L.J., Yin, H.F., Wang, W.G.: Synthesis, characterization, and catalytic activity of Mn-doped perovskite oxides for three-way catalysis. Chem. Eng. Technol. 38(2), 291–296 (2015)CrossRefGoogle Scholar
  9. 9.
    Nishihata, Y., Mizuki, J., Akao, T., Tanaka, H., Uenishi, M., Kimura, M., Okamoto, T., Hamada, N.: Self-regeneration of a Pd-perovskite catalyst for automotive emissions control. Nature. 418(6894), 164–167 (2002)CrossRefGoogle Scholar
  10. 10.
    Tanaka, H., Uenishi, M., Taniguchi, M., Tan, I., Narita, K., Kimura, M., Kaneko, K., Nishihata, Y., Mizuki, J.: The intelligent catalyst having the self-regenerative function of Pd, Rh and Pt for automotive emissions control. Catal. Today. 117(1–3), 321–328 (2006)CrossRefGoogle Scholar
  11. 11.
    Uenishi, M., Tanaka, H., Taniguchi, M., Tan, I., Nishihata, Y., Mizuki, J., Kobayashi, T.: Time evolution of palladium structure change with redox fluctuations in a LaFePdO3 perovskite automotive catalyst by high-speed analysis with in situ DXAFS. Catal. Commun. 9(2), 311–314 (2008)CrossRefGoogle Scholar
  12. 12.
    Keav, S., Matam, S.K., Ferri, D., Weidenkaff, A.: Structured perovskite-based catalysts and their application as three-way catalytic converters - a review. Catalysts. 4(3), 226–255 (2014)CrossRefGoogle Scholar
  13. 13.
    Eyssler, A., Lu, Y., Matam, S.K., Weidenkaff, A., Ferri, D.: Perovskite-supported palladium for methane oxidation - structure-activity relationships. Chimia. 66(9), 675–680 (2012)CrossRefGoogle Scholar
  14. 14.
    Eyssler, A., Mandaliev, P., Winkler, A., Hug, P., Safonova, O., Figi, R., Weidenkaff, A., Ferri, D.: The effect of the state of Pd on methane combustion in Pd-doped LaFeO3. J. Phys. Chem. C. 114(10), 4584–4594 (2010)CrossRefGoogle Scholar
  15. 15.
    Lu, Y., Eyssler, A., Otal, E.H., Matam, S.K., Brunko, O., Weidenkaff, A., Ferri, D.: Influence of the synthesis method on the structure of Pd-substituted perovskite catalysts for methane oxidation. Catal. Today. 208(1), 42–47 (2013)CrossRefGoogle Scholar
  16. 16.
    Mondragón-Rodríguez, G.C., Saruhan, B., Petrova, O., Grünert, W.: Pd-integrated perovskites as effective catalysts for the selective catalytic reduction of NOx with propene. Top. Catal. 52(13–20), 1723–1727 (2009)CrossRefGoogle Scholar
  17. 17.
    Katz, M.B., Graham, G.W., Duan, Y.W., Liu, H., Adamo, C., Schlom, D.G., Pan, X.Q.: Self-regeneration of Pd-LaFeO3 catalysts: new insight from atomic-resolution electron microscopy. J. Am. Chem. Soc. 133(45), 18090–18093 (2011)CrossRefGoogle Scholar
  18. 18.
    Katz, M.B., Zhang, S., Duan, Y., Wang, H., Fang, M., Zhang, K., Li, B., Graham, G.W., Pan, X.: Reversible precipitation/dissolution of precious-metal clusters in perovskite-based catalyst materials: bulk versus surface re-dispersion. J. Catal. 293, 145–148 (2012)CrossRefGoogle Scholar
  19. 19.
    Heikens, S.: Darstellung und Charakterisierung edelmetalldotierter La, Fe, Co-Perowskite als selbstregenerierende Katalysatoren in der Dreiwegekatalyse. PhD Thesis, Ruhr-Universität Bochum, 2014, to be accessed under http://www-brs.ub.ruhr-uni-bochum.de/netahtml/HSS/Diss/HeikensSascha/diss.pdf
  20. 20.
    Saruhan, B., Mondragón Rodríguez, G.C., Haidry, A.A., Yüce, A., Heikens, S., Grünert, W.: Integrated performance monitoring of three-way catalytic converters by self-regenerative and adaptive high-temperature catalyst and sensors. Adv. Eng. Mater. 18(5), 728–738 (2016)CrossRefGoogle Scholar
  21. 21.
    Mondragón-Rodríguez, G.C., Kelm, K., Heikens, S., Grünert, W., Saruhan, B.: Pd-integrated perovskites for TWC application: synthesis, microstructure and N2O selectivity. Catal. Today. 184(1), 184–191 (2012)CrossRefGoogle Scholar
  22. 22.
    Royer, S., Duprez, D.: Catalytic oxidation of carbon monoxide over transition metal oxides. ChemCatChem. 3(1), 24–65 (2011)CrossRefGoogle Scholar
  23. 23.
    Royer, S., Duprez, D., Can, F., Courtois, X., Batiot-Dupeyrat, C., Laassiri, S., Alamdari, H.: Perovskites as substitutes of noble metals for heterogeneous catalysis: dream or reality. Chem. Rev. 114(20), 10292–10368 (2014)CrossRefGoogle Scholar

Copyright information

© Springer Nature Switzerland AG 2019

Authors and Affiliations

  1. 1.Lehrstuhl für Technische ChemieRuhr-Universität BochumBochumGermany
  2. 2.German Aerospace Center, Department of High-temperature and Functional CoatingsInstitute of Materials ResearchCologneGermany

Personalised recommendations

Cite article

Buy options