The [(NH3)4Cu2O2]2+-Peroxo Complex as the Key Intermediate for NH3-SCR Activity and Deactivation of Cu-CHA Catalysts.
Reviewartikel, 2024

In NH3-SCR over Cu-CHA catalysts in the low-temperature range 150–300 °C, the activation of oxygen occurs via oxidation of a pair of mobile (NH3)2CuI-complexes located in the cages of the zeolite. In this step, a reactive [(NH3)4Cu2O2]2+-peroxo complex (μ-η2,η2-peroxo diamino dicopper(II)-complex) is formed. The chemistry of this complex determines several catalytic properties of the Cu-CHA catalyst. The reaction of NO with the [(NH3)4Cu2O2]2+-peroxo complex governs the NH3-SCR activity. A reaction of the [(NH3)4Cu2O2]2+-peroxo complex with ammonia hinders the reaction of NO with the complex, thus leading to an inhibition of the NH3-SCR reaction. Finally, the deactivation in presence of SO2 is due to a reaction of SO2 with the [(NH3)4Cu2O2]2+-peroxo complex, leading to the formation of Cu−S compounds in the catalyst. In this review, the characterization and the reactions of the [(NH3)4Cu2O2]2+-peroxo complex with NO, NH3, and SO2, and mean-field kinetic models based on first principles calculations for NH3-SCR activity and SO2 poisoning are discussed.

Författare

Ton Janssens

Umicore Denmark ApS

Elisa Borfecchia

Universita degli Studi di Torino

Kirill A. Lomachenko

European Synchrotron Radiation Facility (ESRF)

Henrik Grönbeck

Chalmers, Fysik, Kemisk fysik

Kompetenscentrum katalys

Gloria Berlier

Universita degli Studi di Torino

ChemCatChem

1867-3880 (ISSN) 1867-3899 (eISSN)

Vol. 16 18 e202400384

The Competence Centre for Catalysis, KCK 2022-2026

Preem AB (KCK2022-2026), 2022-01-01 -- 2026-12-31.

Johnson Matthey (2500123383), 2022-01-01 -- 2026-12-31.

Volvo Group (PO:2435702-000), 2022-01-01 -- 2026-12-31.

Scania CV AB (Dnr:2021-036543Pnr:52689-1), 2022-01-01 -- 2026-12-31.

Umicore Denmark ApS (KCK2022-2026), 2022-01-01 -- 2026-12-31.

Cu-CHA zeolite-based catalysts for the selective catalytic reduction of NOx in exhaust diesel gas: addressing the issue of Sulfur Stability (CHASS)

Europeiska kommissionen (EU) (EC/H2020/955839), 2021-06-01 -- 2025-05-31.

Ämneskategorier

Oorganisk kemi

Fysikalisk kemi

Organisk kemi

DOI

10.1002/cctc.202400384

Mer information

Senast uppdaterat

2024-10-07