Litcius/Paper detail

Mechanism of Standard NH<sub>3</sub>–SCR over Cu-CHA via NO<sup>+</sup> and HONO Intermediates

Chong Liu, Shunsaku Yasumura, Takashi Toyao, Zen Maeno, Ken‐ichi Shimizu

2022The Journal of Physical Chemistry C25 citationsDOI

Abstract

The mechanism of the selective catalytic reduction of NO by NH3 (NH3–SCR) over Cu-CHA zeolite was investigated by in situ/operando IR experiments collaborated with density functional theory (DFT) calculations. Operando IR experiments under transient conditions show the formation of NO+ intermediate and its reaction with NH3. DFT calculations suggest that the reduction half-cycle of NH3–SCR occurs via NO+/HONO intermediates with Cu sites and Brønsted acid sites (BASs) both playing important roles. In the proposed reduction half-cycle, the CuII sites are responsible for the activation of NO into NO+/HONO intermediates, which then react with NH3 to afford N2 and H2O over BASs.

Topics & Concepts

Density functional theoryCatalytic cycleChemistryCatalysisReaction mechanismReaction intermediateZeoliteReactive intermediateSelective catalytic reductionBass (fish)Brønsted–Lowry acid–base theoryPhotochemistryAmmoniaInorganic chemistryComputational chemistryOrganic chemistryEcologyBiologyCatalytic Processes in Materials ScienceAmmonia Synthesis and Nitrogen ReductionNanomaterials for catalytic reactions