Unexpected promotional effects of HCl over CeO2-based catalysts for NOx reduction against alkali poisoning

Abstract

In the flue gas of stationary NOx emission source, HCl was deemed to be one of the poisons of NOx reduction catalysts since it can react with ammonia to form NH4Cl and adhere to oxide surface, reducing the redox property and blocking the active sites of catalysts for selective catalytic reduction of NOx with NH3 (NH3-SCR). Herein, unexpected promotional effects of HCl over CeO2-based catalysts for NOx reduction against alkali poisoning have been unraveled. The modification of gaseous HCl on the surface of CeO2 constructed Cl-Ce-O-Ce-OH and Cl-Ce-O-Ce3+ sites, providing additional Brønsted and Lewis acid sites to facilitate ammonia adsorption. It is worth noting that HCl can not only directly neutralize alkali metal to reduce alkalinity, but also increase the acidity to offset the encroachment of acid sites by alkali metal poisoning. The lower NO adsorption energy and weaker oxidation property of Cl-Ce-O-Ce3+ sites also prevented the accumulation of inert nitrate on the surface of alkali metal poisoned catalyst. This work unveils multi-promotion mechanisms for the enhanced catalytic activity and anti-alkali poisoning of gaseous HCl modified cerium-based NOx reduction catalysts, providing a new thinking based on pollutant interaction for further development of highly efficient NOx reduction catalysts in multipollutant flue gas.