Abstract
Herein, we demonstrated the selective catalytic oxidation of diethylamine to N2 over MnOx/ZSM-5 catalysts. It was found that oxidation activity of diethylamine over MnOx/ZSM-5 catalysts increased when the loading of Mn increased, but the N2 selectivity decreased at 420 °C obviously. MnOx/ZSM-5(360) catalysts showed higher oxidation activity of diethylamine than MnOx/ZSM-5(18) catalysts with equivalent Mn loading, which was ascribed to the presence of MnOx species easily reduced and enriched on ZSM-5(360) support surface. However, MnOx/ZSM-5(18) catalysts containing moderate and strong surface acid centers in addition to the weak acid centers gave significantly higher N2 selectivity than MnOx/ZSM-5(360) catalysts possessing only weak surface acid centers. 20MnOx/ZSM-5(18) catalyst had relatively high oxidation activity of diethylamine and N2 selectivity, of which the lowest reaction temperature for diethylamine conversion at 98% (T98) is 240 °C and the N2 selectivity is exceeding 95.5% at 420 °C. Furthermore, 20MnOx/ZSM-5(18) catalyst showed wider temperature window (ΔT = 180 °C) with N2 selectivity over 95% than 20MnOx/ZSM-5(360) catalyst (ΔT = 80 °C). It can be concluded that the easily reduced and surface enriched MnOx species are favorable for the oxidation of diethylamine, the moderate and strong surface acid centers are beneficial to activation of diethylamine and the generation of N2.
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