Kinetic Monte Carlo Simulations of Low‐Temperature NH₃‐SCR over Cu‐Exchanged Chabazite

Cu‐exchanged chabazite (Cu‐CHA) is widely used for ammonia assisted selective catalytic reduction of nitrogen oxides (NH 3 ‐SCR). The Cu + ions are at low temperatures solvated by NH 3 forming mobile [Cu(NH 3 ) 2 ] + complexes. The dynamic behaviour of the complexes is critical as O 2 adsorption requires a pair of complexes to form a [Cu 2 (NH 3 ) 4 O 2 ] 2+ peroxo‐species over which NO couples with NH 3 . Here we introduce a first principles‐based kinetic Monte Carlo approach to explore the effect of the Al‐distribution on the reaction kinetics of NH 3 ‐SCR over Cu‐CHA. The method allows us to scrutinize the interplay between the pairing of [Cu(NH 3 ) 2 ] + complexes and the reaction landscape for the NH 3 ‐SCR reaction over the peroxo‐complex. The Al‐distribution affects the stability of the [Cu(NH 3 ) 2 ] + pairs as well as the kinetic parameters of the SCR‐reaction. The turn‐over frequency is determined by the stability of the [Cu(NH 3 ) 2 ] + pairs and the relative strength of NO and NH 3 adsorption once a pair is present. The results establish the hierarchy of effects that influences the performance of Cu‐CHA over NH 3 ‐SCR and provide a computational basis for further development of the Cu‐CHA material.