Constructing Bridge Hydroxyl Groups on the Ru/MOx/HZSM-5 (M = W, Mo) Catalysts to Promote the Hydrolysis Oxidation of Multicomponent VOCs

Environ Sci Technol. 2024 Dec 24. doi: 10.1021/acs.est.4c09649. Online ahead of print.

Abstract

Chlorinated and oxygenated volatile organic compounds (CVOCs and OVOCs) pose a significant threat to human health. Catalytic oxidation effectively removes these pollutants, but catalyst deactivation is a challenge. Our study focused on the hydrolysis oxidation of chlorobenzene (CB) and ethyl acetate (EA) over Ru/MOx/HZSM-5 (M = W, Mo). It was found that doping MoOx to the catalyst increased the structural hydroxyl amount and balanced surface acidity, thus significantly improving the catalytic stability, with Ru/MoOx/HZSM-5 exhibiting a better activity for CB and EA oxidation (T90% = 438 and 276 °C at space velocity = 20,000 mL g-1 h-1, respectively). Water vapor introduction considerably promoted hydrolysis oxidation and protected the active sites from being poisoned by cumulative chlorine. The synergistic interaction of the Mo-O(H)-Al structure in Ru/MoOx/HZSM-5 with the Si-OH-Al structure promotes the activation of H2O to form bridging hydroxyl groups, which provide a proton-rich environment for hydrolysis oxidation. It was also found that dissociated H2O reacted with adsorbed oxygen species to form highly active *OOH, accelerating the deep oxidation of intermediates. We believe that the present study can provide a unique strategy for the effective elimination of multicomponent VOCs under complex conditions.

Keywords: HZSM-5-supported Ru catalyst; bridging hydroxyl groups; hydrolysis oxidation; volatile organic compound; water vapor promotion.