Cu‐SSZ‐13 Catalysts Designed Through Interzeolite Conversion Process From Different Structure Types of Zeolites for NH 3 ‐SCR‐DeNO x : Structure‐Property Activity Relationships and Intermediates Determination

ChemCatChem, vol. 17

Abstract

Abstract The intermediates and their respective role in reduction and oxidation cycles in the selective catalytic reduction of NO xx with ammonia reaction mechanism (NH 3 ‐SCR‐DeNO x ) are widely and controversially discussed. To finally clear up the discussion, a variety of Cu‐containing CHA structure type zeolites (Cu‐SSZ‐13) were prepared using different zeolite sources, such as MFI, BEA and FAU structure type zeolites. Cu‐SSZ‐13 prepared samples were investigated as catalysts for NH 3 ‐SCR‐DeNO x . The structure‐property‐activity relationship of the Cu‐SSZ‐13 prepared samples varied depending on the applied initial zeolite. Cu‐SSZ‐13 catalysts prepared from MFI and BEA structure types of zeolites are more N 2 selective than Cu‐SSZ‐13 catalysts prepared from FAU structure type of zeolite. In situ spectroscopy, temperature‐programmed and transient techniques supported by density functional theory (DFT) were used to investigate the reaction mechanism and confirmed the intermediates of the reduction‐ and oxidation‐half cycles: NH 4 + , NH x − , [(NH 3 ) 4 Cu II 2 O 2 ] 2+ , NO 2 − /NO 3 − species. The SCR paths involved determine that the dominant reaction occurs between adsorbed NH 3 on the catalyst surface and NO from the gas phase, as well as the reaction between adsorbed NO x − (nitrites/nitrates) and NH 3 .

Authors 14

1. Alejandro Mollá Robles

   Leipzig University

   Affiliation as printed

   Institute of Chemical Technology Universität Leipzig Linnéstr. 3 04103 Leipzig Germany

2. Magdalena Jabłońska corresponding

   Leipzig University

   Affiliation as printed

   Institute of Chemical Technology Universität Leipzig Linnéstr. 3 04103 Leipzig Germany

3. Ana Palčić

   Ruđer Bošković Institute

   Affiliation as printed

   Laboratory for the Synthesis of New Materials Division of Materials Chemistry Ruđer Bošković Institute Bijenička 54 Zagreb 10000 Croatia

4. Matej Bubaš

   National Institute of Chemistry

   Affiliation as printed

   Laboratory for Catalysts Department of Inorganic Chemistry and Technology National Institute of Chemistry Ljubljana SI‐1000 Slovenia

   Laboratory for Catalysts, Department of Inorganic Chemistry and Technology, National Institute of Chemistry, Ljubljana, SI-1000 Slovenia

5. Jie Yang

   Wuhan Textile University

   Affiliation as printed

   Hubei Key Laboratory of Biomass Fibers and Eco‐dyeing and Finishing College of Chemistry and Chemical Engineering Wuhan Textile University Wuhan 430200 China

   Hubei Key Laboratory of Biomass Fibers and Eco-dyeing and Finishing, College of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200 China

6. Marek Rotko

   Maria Curie-Skłodowska University

   Affiliation as printed

   Department of Chemical Technology Institute of Chemical Sciences Faculty of Chemistry Maria Curie‐Sklodowska University 3 Maria Curie‐Sklodowska Sq. Lublin 20031 Poland

   Department of Chemical Technology, Institute of Chemical Sciences, Faculty of Chemistry, Maria Curie-Sklodowska University, 3 Maria Curie-Sklodowska Sq., Lublin, 20031 Poland

7. Muhammad Fernadi Lukman

   Leipzig University

   Affiliation as printed

   Felix Bloch Institute for Solid State Physics Universität Leipzig Linnéstr. 5 04103 Leipzig Germany

8. Anqi Guo Aachen Institute of Inorganic Chemistry

   RWTH Aachen University

   Affiliation as printed

   Institute of Inorganic Chemistry RWTH Aachen University 52074 Aachen Germany

   Institute of Inorganic Chemistry, RWTH Aachen University, 52074 Aachen, Germany

9. Marko Bertmer

   Leipzig University

   Affiliation as printed

   Felix Bloch Institute for Solid State Physics Universität Leipzig Linnéstr. 5 04103 Leipzig Germany

10. Matej Huš

    National Institute of Chemistry

    Affiliation as printed

    Department of Catalysis and Chemical Reaction Engineering National Institute of Chemistry Ljubljana SI‐1000 Slovenia

    Department of Catalysis and Chemical Reaction Engineering, National Institute of Chemistry, Ljubljana, SI-1000 Slovenia

11. Junjiang Zhu

    Wuhan Textile University

    Affiliation as printed

    Hubei Key Laboratory of Biomass Fibers and Eco‐dyeing and Finishing College of Chemistry and Chemical Engineering Wuhan Textile University Wuhan 430200 China

    Hubei Key Laboratory of Biomass Fibers and Eco-dyeing and Finishing, College of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200 China

12. Ulrich Simon Aachen Institute of Inorganic Chemistry

    RWTH Aachen University

    Affiliation as printed

    Institute of Inorganic Chemistry RWTH Aachen University 52074 Aachen Germany

    Institute of Inorganic Chemistry, RWTH Aachen University, 52074 Aachen, Germany

13. Andreas Pöppl

    Leipzig University

    Affiliation as printed

    Felix Bloch Institute for Solid State Physics Universität Leipzig Linnéstr. 5 04103 Leipzig Germany

14. Nataša Novak Tušar

    National Institute of Chemistry

    Affiliation as printed

    Laboratory for Catalysts Department of Inorganic Chemistry and Technology National Institute of Chemistry Ljubljana SI‐1000 Slovenia

    Laboratory for Catalysts, Department of Inorganic Chemistry and Technology, National Institute of Chemistry, Ljubljana, SI-1000 Slovenia