Efficacious destruction of typical aromatic hydrocarbons over CoMn/Ni foam monolithic catalysts with boosted activity and water resistance

J Colloid Interface Sci. 2024 Aug 15:668:98-109. doi: 10.1016/j.jcis.2024.04.165. Epub 2024 Apr 24.

Abstract

Developing cost-effective monolith catalyst with superior low-temperature activity is critical for oxidative efficacious removal of industrial volatile organic compounds (VOCs). However, the complexity of the industrial flue gas conditions demands the need for high moisture tolerance, which is challenging. Herein, CoMn-Metal Organic Framework (CoMn-MOF) was in situ grown on Ni foam (NiF) at room temperature to synthesize the cost-effective monolith catalyst. The optimized catalyst, Co1Mn1/NiF, exhibited excellent performance in toluene oxidation (T90 = 239 °C) due to the substitution of manganese into the cobalt lattice. This substitution weakened the Co-O bond strength, creating more oxygen vacancies and increasing the active oxygen species content. Additionally, experimentally and computationally evidence revealed that the mutual inhibiting effect of three typical aromatic hydrocarbons (benzene, toluene and m-xylene) over the Co1Mn1/NiF catalyst was attributed to the competitive adsorption occurring on the active site. Furthermore, the Co1Mn1/NiF catalyst also presents outstanding water resistance, particularly at a concentration of 3 vol%, where the activity is even enhanced. This was attributed to the lower water adsorption and dissociation energy derived from the interaction between the bimetals. Results demonstrate that the dissociation of water vapor enables more reactive oxygen species to participate in the reaction which reduces the formation of intermediates and facilitates the reaction. This investigation provides new insights into the preparation of oxygen vacancy-rich monolith catalysts with high water resistance for practical applications.

Keywords: Aliovalent substitution; Monolith catalyst; Oxygen vacancy; VOC oxidation; Water resistance.