Influence of aluminium distribution on the diffusion mechanisms and pairing of [Cu(NH3)2]+ complexes in Cu-CHA
Artikel i vetenskaplig tidskrift, 2025

The performance of Cu-exchanged chabazite (Cu-CHA) for the ammonia-assisted selective catalytic reduction of NOx (NH3-SCR) depends critically on the presence of paired formula presented complexes. Here, a machine-learning force field augmented with long-range Coulomb interactions is developed to investigate the effect of Al-distribution and Cu-loading on the mobility and pairing of formula presented complexes. Performing unbiased and constrained molecular dynamics simulations, we obtain unique information inaccessible to first-principle calculations and experiments. The free energy barrier for formula presented diffusion between CHA-cages depends sensitively on both the local and distant Al-distribution. Importantly, certain Al-distributions and arrangements of neighboring formula presented cations make paired formula presented complexes exothermic with respect to separated configurations. Our results suggest that the NH3-SCR activity can be enhanced by increasing the Cu-loading and Al-content. The dynamic interplay between formula presented diffusion is crucial for the formula presented mobility and stresses the need to explore large systems including long-range Coulomb interactions when studying diffusion of charged species in zeolites.

Författare

Joachim Bjerregaard

Umicore Denmark ApS

Chalmers, Fysik, Kemisk fysik

Martin Votsmeier

Umicore Denmark ApS

Henrik Grönbeck

Chalmers, Fysik, Kemisk fysik

Nature Communications

2041-1723 (ISSN) 20411723 (eISSN)

Vol. 16 1 603-

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.

The Competence Centre for Catalysis, KCK 2022-2026

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

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

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

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

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

Ämneskategorier (SSIF 2025)

Organisk kemi

Fysikalisk kemi

Infrastruktur

Chalmers e-Commons (inkl. C3SE, 2020-)

DOI

10.1038/s41467-025-55859-1

PubMed

39799150

Relaterade dataset

Influence of aluminium distribution on the diffusion mechanisms and pairing of [Cu(NH3)2]+ complexes in Cu-CHA [dataset]

URI: https://doi.org/10.5281/zenodo.14290247

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Senast uppdaterat

2025-01-29