Isolated copper ions exchanged onto zeolites catalyze the selective reduction of nitrogen oxides with ammonia in the presence of excess dioxygen. We present evidence that the mechanism of catalytic action at low temperatures, conditions in which copper ions are fully coordinated and solvated by ammonia, involves the dynamic formation of binuclear cuprous amine complexes to activate dioxygen during oxidation half-cycles. We discuss the catalytic consequences of ionic tethering of cationic transition metal complexes at anionic framework aluminum centers in zeolites, which enables the reversible formation of multinuclear sites from mobilized single sites and provides energetically-favorable pathways to utilize dioxygen in partial oxidation catalysis at low temperatures.

Mechanistic consequences of Cu ion mobility in zeolites for the selective catalytic reduction of nitrogen oxides with ammonia

255th National Meeting (2018)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.