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AdSCR Systems (Adsorption + Selective Catalytic Reduction): Analysis of the Influence of H2O and CO2 on Low Temperature NOx Emission Reduction Performances

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Abstract

The removal of NOx from low-temperature diesel engine emissions still represents a big challenge in view of the upcoming more stringent worldwide regulations. In our previous studies, we proved the ability of novel AdSCR (Adsorption + Selective Catalytic Reduction) systems, based on the combination of a chemical trap** compound and a conventional SCR catalyst, to trap cold start NOx emissions and to desorb and simultaneously reduce them with ammonia at higher temperature. In the present work, we extend the investigation of Cu-CHA + BaO/Al2O3 systems under more realistic conditions, focusing on the impact of H2O and CO2. The experimental results reveal a reduction of the AdSCR system performances with respect to dry and CO2-free conditions. Despite this, the system is still able to store and reduce NOx. The NOx storage capacity on barium oxide is more affected by the presence of CO2 than by H2O. However, H2O hinders the NO oxidative activation in the zeolite cages, which is a fundamental step in order to be able to trap NOx on the storage material at low temperature. We further demonstrate that the detrimental effect of H2O can be mitigated by small amounts of NO2 in the gaseous feed or by including a 13X zeolite guard bed prior to the AdSCR bed.

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References

  1. Seykens, X., Kupper, F., Mentink, P., Ramesh, S.: Towards ultra-low NOx emissions within GHG Phase 2 constraints: main challenges and technology directions. SAE Tech. Pap. 1–14 (2018).

  2. Nova, I., Tronconi, E.: Urea-SCR technology for deNOx after tretment of diesel exhausts. Springer-Verlag, New York (2014)

    Book  Google Scholar 

  3. Brandenberger, S., Kröcher, O., Tissler, A., Althoff, R.: The state of the art in selective catalytic reduction of NOx by ammonia using metal-exchanged zeolite catalysts. Catal. Rev.: Sci. Eng. 50, 492–531 (2008)

    Article  Google Scholar 

  4. Dahodwala, M., Joshi, S., Koehler, E.W., Franke, M., Tomazic, D.: Strategies for meeting phase 2 GHG and ultra-low NOx emission standards for heavy-duty diesel engines. SAE Int. J. Engines. 11, 1109–1122 (2018)

    Article  Google Scholar 

  5. Theis, J.R., Lambert, C.K.: Mechanistic assessment of low temperature NOx adsorbers for cold start NOx control on diesel engines. Catal. Today. 320, 181–195 (2019)

    Article  Google Scholar 

  6. Koebel, M., Elsener, M., Madia, G.: Reaction pathways in the selective catalytic reduction process with NO and NO2 at low temperatures. Ind. Eng. Chem. Res. 40, 52–59 (2001)

    Article  Google Scholar 

  7. Birkhold, F., Meingast, U., Wassermann, P., Deutschmann, O.: Modeling and simulation of the injection of urea-water-solution for automotive SCR DeNOx-systems. Appl. Catal. B Environ. 70, 119–127 (2007)

    Article  Google Scholar 

  8. Ji, Y., Bai, S., Crocker, M.: Al2O3-based passive NOx adsorbers for low temperature applications. Appl. Catal. B Environ. 170–171, 283–292 (2015)

    Article  Google Scholar 

  9. Chen, H.Y., Collier, J.E., Liu, D., Mantarosie, L., Durán-Martín, D., Novák, V., Rajaram, R.R., Thompsett, D.: Low temperature NO storage of zeolite supported Pd for low temperature diesel engine emission control. Catal. Letters. 146, 1706–1711 (2016)

    Article  Google Scholar 

  10. Khivantsev, K., Jaegers, N.R., Kovarik, L., Prodinger, S., Derewinski, M.A., Wang, Y., Gao, F., Szanyi, J.: Palladium/Beta zeolite passive NOx adsorbers (PNA): Clarification of PNA chemistry and the effects of CO and zeolite crystallite size on PNA performance. Appl. Catal. A Gen. 569, 141–148 (2019)

    Article  Google Scholar 

  11. Kim, M.S., Lee, D.W., Chung, S.H., Hong, Y.K., Lee, S.H., Oh, S.H., Cho, I.H., Lee, K.Y.: Oxidation of ammonia to nitrogen over Pt/Fe/ZSM5 catalyst: influence of catalyst support on the low temperature activity. J. Hazard. Mater. 237–238, 153–160 (2012)

    Article  Google Scholar 

  12. Wang, A., **e, K., Kumar, A., Kamasamudram, K., Olsson, L.: Layered Pd/SSZ-13 with Cu/SSZ-13 as PNA − SCR dual-layer monolith catalyst for NOx abatement. Catal. Today. 360, 356–366 (2021)

    Article  Google Scholar 

  13. Selleri, T., Gramigni, F., Nova, I., Tronconi, E., Dieterich, S., Weibel, M., Schmeisser, V.: A PGM-free NOx adsorber + Selective Catalytic Reduction catalyst system (AdSCR) for trap** and reducing NOx in lean exhaust streams at low temperature. Catal. Sci. Technol. 8, 2467–2476 (2018)

    Article  Google Scholar 

  14. Gramigni, F., Selleri, T., Nova, I., Tronconi, E., Dieterich, S., Weibel, M., Schmeisser, V.: Analysis of AdSCR systems for NOx removal during the cold-start period of diesel engines. Top. Catal. 62, 3–9 (2019)

    Article  Google Scholar 

  15. Gramigni, F., Nasello, N.D., Selleri, T., Nova, I., Tronconi, E., Dieterich, S., Weibel, M.: Unexpected low-temperature deNOx activity of AdSCR systems for cold start NOx abatement. Emiss. Control Sci. Technol. 6, 402–409 (2020)

    Article  Google Scholar 

  16. Selleri, T., Ruggeri, M.P., Nova, I., Tronconi, E.: The low temperature interaction of NO + O2 with a commercial Cu-CHA Catalyst: a chemical trap** study. Top. Catal. 59, 678–685 (2016)

    Article  Google Scholar 

  17. Ruggeri, M.P., Selleri, T., Nova, I., Tronconi, E., Pihl, J.A., Toops, T.J., Partridge, W.P.: New mechanistic insights in the NH3-SCR reactions at low temperature. Top. Catal. 59, 907–912 (2016)

    Article  Google Scholar 

  18. Ruggeri, M.P., Selleri, T., Colombo, M., Nova, I., Tronconi, E.: Identification of nitrites/HONO as primary products of NO oxidation over Fe-ZSM-5 and their role in the standard SCR mechanism: a chemical trap** study. J. Catal. 311, 266–270 (2014)

    Article  Google Scholar 

  19. Gramigni, F., Selleri, T., Nova, I., Tronconi, E.: Catalyst systems for selective catalytic reduction + NOx trap**: from fundamental understanding of the standard SCR reaction to practical applications for lean exhaust after-treatment. React. Chem. Eng. 4, 1165–1178 (2019)

    Article  Google Scholar 

  20. Lietti, L., Daturi, M., Blasin-Aubé, V., Ghiotti, G., Prinetto, F., Forzatti, P.: Relevance of the nitrite route in the NOx adsorption mechanism over Pt-Ba/Al2O3 NOx storage reduction catalysts investigated by using operando FTIR spectroscopy. ChemCatChem 4, 55–58 (2012)

    Article  Google Scholar 

  21. Nova, I., Castoldi, L., Lietti, L., Tronconi, E., Forzatti, P., Prinetto, F., Ghiotti, G.: NOx adsorption study over Pt-Ba/alumina catalysts: FT-IR and pulse experiments. J. Catal. 222, 377–388 (2004)

    Article  Google Scholar 

  22. Ciardelli, C., Nova, I., Tronconi, E., Chatterjee, D., Bandl-Konrad, B.: A “Nitrate Route” for the low temperature “Fast SCR” reaction over a V2O5-WO3/TiO2 commercial catalyst. Chem. Commun. 20133, 2718–2719 (2004)

    Article  Google Scholar 

  23. Tronconi, E., Nova, I., Ciardelli, C., Chatterjee, D., Bandl-Konrad, B., Burkhardt, T.: Modelling of an SCR catalytic converter for diesel exhaust after treatment: dynamic effects at low temperature. Catal. Today. 105, 529–536 (2005)

    Article  Google Scholar 

  24. Schmeisser, V., Weibel, M., Sebastian Hernando, L., Nova, I., Tronconi, E., Ruggeri, M.P.: Cold start effect phenomena over zeolite SCR catalysts for exhaust gas aftertreatment. SAE Int. J. Commer. Veh. 6, 190–199 (2013)

    Article  Google Scholar 

  25. Tao, T., **e, Y., Dawes, S., Melscoet-chauvel, I., Pfeifer, M., Spurk, P.C., Ag, U., Kg, C.: Diesel SCR NOx reduction and performance on washcoated SCR catalysts. SAE Tech. P. 2004–01–1293 (2004).

  26. Weiss, B.M., Caldwell, K.B., Iglesia, E.: NOx interactions with dispersed BaO: adsorption kinetics, chemisorbed species, and effects of oxidation catalyst sites. J. Phys. Chem. C 115, 6561–6570 (2011)

    Article  Google Scholar 

  27. Selleri, T., Nova, I., Tronconi, E.: The low-temperature interaction of NH3/NO/NO2 + O2 with Fe-ZSM-5 + BaO/Al2O3 and H-ZSM-5 + BaO/Al2O3: influence of phase separation and relevance for the NH3-SCR chemistry. Appl. Catal. B Environ. 206, 471–478 (2017)

    Article  Google Scholar 

  28. Ruggeri, M.P., Selleri, T., Colombo, M., Nova, I., Tronconi, E.: Investigation of NO2 and NO interaction with an Fe-ZSM-5 catalyst by transient response methods and chemical trap** techniques. J. Catal. 328, 258–269 (2015)

    Article  Google Scholar 

  29. Epling, W.S., Campbell, G.C., Parks, J.E.: The effects of CO2 and H2O on the NOx destruction performance of a model NOx storage/reduction catalyst. Catal. Letters. 90, 45–56 (2003)

    Article  Google Scholar 

  30. Tutuianu, M., Inderwildi, O.R., Bessler, W.G., Warnatz, J.: Competitive adsorption of NO, NO2, CO2, and H2O on BaO(100): a quantum chemical study. J. Phys. Chem. B. 110, 17484–17492 (2006)

    Article  Google Scholar 

  31. Tatlier, M., Munz, G., Henninger, S.K.: Relation of water adsorption capacities of zeolites with their structural properties. Microporous Mesoporous Mater. 264, 70–75 (2018)

    Article  Google Scholar 

  32. Maestri, M., Iglesia, E.: First-principles theoretical assessment of catalysis by confinement: NO-O2 reactions within voids of molecular dimensions in siliceous crystalline frameworks. Phys. Chem. Chem. Phys. 20, 15725–15735 (2018)

    Article  Google Scholar 

  33. Artioli, N., Lobo, R.F., Iglesia, E.: Catalysis by confinement: enthalpic stabilization of NO oxidation transition states by micropororous and mesoporous siliceous materials. J. Phys. Chem. C. 117, 20666–20674 (2013)

    Article  Google Scholar 

  34. Bendrich, M., Scheuer, A., Votsmeier, M.: Importance of nitrates in Cu-SCR modelling: a validation study using different driving cycles. Catal. Today. 360, 252–262 (2021)

    Article  Google Scholar 

  35. Cort, B., Chejne, F., Carrasco, F., Moreno, C.: Water adsorption on zeolite 13X: comparison of the two methods based on mass spectrometry and thermogravimetry. Adsorption 16, 141–146 (2010)

    Article  Google Scholar 

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Acknowledgements

The authors acknowledge Dr. Simone Dieterich and Dr. Michel Weibel for important discussions and helpful suggestions.

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This work was financially supported by Mercedes-Benz AG.

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Correspondence to Enrico Tronconi.

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Nasello, N.D., Gramigni, F., Nova, I. et al. AdSCR Systems (Adsorption + Selective Catalytic Reduction): Analysis of the Influence of H2O and CO2 on Low Temperature NOx Emission Reduction Performances. Emiss. Control Sci. Technol. 7, 223–231 (2021). https://doi.org/10.1007/s40825-021-00204-3

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