Correlation of the changes in the framework and active Cu sites for typical Cu/CHA zeolites (SSZ-13 and SAPO-34) during hydrothermal aging

Abstract

The relative framework stability of Cu/CHA zeolites (SAPO-34 and SSZ-13) was studied during hydrothermal aging at 800 °C, and the fundamental mechanism for the framework change was investigated. Additionally, the relationship between the variation in the framework and active SCR reaction sites was established. SAPO-34 showed stronger stability during hydrothermal aging than SSZ-13. The results showed that dealumination occurred in the SSZ-13 zeolite, leading to the loss of crystallinity and a severe decrease of the Brönsted acid sites. Simultaneously, the detached Al(OH)₃ species deactivated the Cu species by the transformation of isolated Cu²⁺ ions to CuAlO_x species. While the vacancy in the SAPO-34 framework caused by desilication could be healed with the migration of extra-framework Al and P atoms to the defects. And the Cu species showed a certain degree of aggregation with the improved redox ability of the aged Cu/SAPO-34 zeolite and the acidic properties were well maintained.