Determining the storage, availability and reactivity of NH₃ within Cu-Chabazite-based Ammonia Selective Catalytic Reduction systems

Three different types of NH₃ species can be simultaneously present on Cu2+-exchanged CHA-type zeolites, commonly used in Ammonia Selective Catalytic Reduction (NH₃-SCR) systems. These include ammonium ions (NH4+), formed on the Brønsted acid sites, [Cu(NH₃)4]2+ complexes, resulting from NH₃ coordination with the Cu2+ Lewis sites, and NH₃ adsorbed on extra-framework Al (EFAl) species, in contrast to the only two reacting NH₃ species recently reported on Cu-SSZ-13 zeolite. The NH4+ ions react very slowly in comparison to NH₃ coordinated to Cu2+ ions and are likely to contribute little to the standard NH₃-SCR process, with the Brønsted groups acting primarily as NH₃ storage sites. The availability/reactivity of NH4+ ions can be however, notably improved by submitting the zeolite to repeated exchanges with Cu2+, accompanied by a remarkable enhancement in the low temperature activity. Moreover, the presence of EFAl species could also have a positive influence on the reaction rate of the available NH4+ ions. These results have important implications for NH₃ storage and availability in Cu-Chabazite-based NH₃-SCR systems.