Ting, RZF; (2017) Computational study of de-NOx reactions in Cu-exchanged zeolites. Doctoral thesis , UCL (University College London).

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Abstract

Copper-exchanged zeolites have been widely studied as catalysts for NOx emission control since the early 1980s. Over the last 40 years, there has been a growing search for a “de-NOx” catalyst in order to reduce and control NOx emissions. Selective catalytic reduction (SCR) is a commonly used method for NOx removal, via catalytic reaction of the nitrogen oxides with ammonia or light hydrocarbons such as propane to produce N2 as the only N-containing product. Cu-exchanged zeolite hosts SSZ-13 and SAPO-34, both belonging to the small-pore CHA framework have high activity in site-resolved de-NOx SCR. The exact nature of the active Cu species and the atomic-level mechanism of the de-NOx reaction are still subject to debate, and are of difficult characterisation by the application of experimental techniques alone. In this thesis the aim is to apply atomistic modelling techniques using both force-field and quantum chemical calculations, the following results has been observed: (i) site SI is the global energy minimum by on average 0.9eV, (ii) the proximity of dopant atoms has a pronounced effect on the equilibrium energy of the system, (iii) H2O and NH3 adsorption is preferable in site SIV and (iv) SAPO-34 is a more reactive system in terms of hosting small polar molecules.

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