SO2-Tolerant Selective Catalytic Reduction of NO x over Meso-TiO2@Fe2O3@Al2O3 Metal-Based Monolith Catalysts.

Abstract

It is an intractable issue to improve the low-temperature SO2-tolerant selective catalytic reduction (SCR) of NO x with NH3 because deposited sulfates are difficult to decompose below 300 °C. Herein, we established a low-temperature self-prevention mechanism of mesoporous-TiO2@Fe2O3 core-shell composites against sulfate deposition using experiments and density functional theory. The mesoporous TiO2-shell effectively restrained the deposition of FeSO4 and NH4HSO4 because of weak SO2 adsorption and promoted NH4HSO4 decomposition on the mesoporous-TiO2. The electron transfer at the Fe2O3 (core)-TiO2 (shell) interface accelerated the redox cycle, launching the "Fast SCR" reaction, which broadened the low-temperature window. Engineered from the nano- to macro-scale, we achieved one-pot self-installation of mesoporous-TiO2@Fe2O3 composites on the self-tailored AlOOH@Al-mesh monoliths. After the thermal treatment, the mesoporous-TiO2@Fe2O3@Al2O3 monolith catalyst delivered a broad window of 220-420 °C with NO conversion above 90% and had superior SO2 tolerance at 260 °C. The effective heat removal of Al-mesh monolithcatalysts restrained NH3 oxidation to NO and N2O while suppressing the decomposition of NH4NO3 to N2O, and this led to much better high-temperature activity and N2 selectivity. This work supplies a new point for the development of low-temperature SO2-tolerant monolithic SCR catalysts with high N2 selectivity, which is of great significance for both academic interests and practical applications.