4.7 Article

Low-temperature catalytic performance of toluene oxidation over Cu-Mn oxide catalysts derived from LDH precursor

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FUEL
卷 347, 期 -, 页码 -

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ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2023.128401

关键词

Layered double hydroxide; Copper-manganese oxides; Low-temperature catalytic oxidation; Toluene; In-situ Diffuse Reflectance Infrared Fourier; Transform Spectroscopy

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A series of CuMn mixed oxides catalysts (CMO-T) were prepared from CuMn layered double hydroxides (CuMn-LDH) and showed high catalytic activity and stability in the oxidation of toluene. The formation of a copper-manganese solid solution with abundant multiple-phase interfaces and the strong interaction between Cu and Mn contributed to the enhanced performance. The facile method of preparing mixed-metal solid solutions from LDH precursors has potential applications in catalytic oxidation.
A series of CuMn mixed oxides catalysts (CMO-T) were prepared by calcination of CuMn layered double hy-droxides (CuMn-LDH) for catalytic oxidation of toluene. The obtained CMO-400 catalyst exhibited a high cat-alytic activity with T50 and T90 of 210 and 231 degrees C (WHSV = 30000 mL center dot g- 1 center dot h-1). Meanwhile, the CMO-400 exhibited high stability and durability even at 20 vol% water vapor. The effects of calcination temperature on the texture and structural properties were investigated systematically, which proved the formation of copper-manganese solid solution with abundant multiple-phase interfaces. In addition, the strong interaction between Cu and Mn could lead to more surface adsorbed oxygen due to oxidation reduction cycle of Mn3++Cu2+=Mn4++Cu+. Accordingly, for CMO-500 catalyst, the formation of spinel Cu1.5Mn1.5O4 phase pre-vented good dispersion of the manganese-oxide phases and weakened the reducibility and oxygen mobility. In-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) revealed that the intermediates accumulated continuously were difficult to be oxidized rapidly without the replenishment gaseous oxygen. Moreover, the complete transformation of the intermediate benzoate may be the key rate-controlling step in the reaction. The Facile method of preparing mixed-metal solid solution from LDH precursor system could be widely developed for the design of transition metals in catalytic oxidation of toluene.

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