Chinese Journal of Chemical Engineering, Vol.28, No.10, 2542-2548, 2020
Highly dispersed metal incorporated hexagonal mesoporous silicates for catalytic cyclohexanone oxidation to adipic acid
Adipic add is a dicarboxylic add of great industrial importance, mainly used in the production of nylon-6,6 and polyurethane. The use of nitric add as an oxidant in the industrial production of adipic acid poses significant carbon footprint to the environment. Clean adipic add synthesis methods using a heterogeneous catalyst with H2O2 as oxidant and water as solvent have potential advantages of low catalyst cost, easy synthesis and recovery, cleanness and environmental protection. In this work, hexagonal mesoporous silicate materials were synthesized by a sot-gel method and evaluated for cyclohexanol/cyclohexanone oxidation to adipic acid. The physical and chemical properties of Fe-HMS were characterized by XRD, HR-TEM, BET and UV-Vis. The experimental results showed that Fe-HMS materials show pore sizes ranging from 2-3 nm. W- and Mo-based polyoxometalates were also evaluated and compared to the Fe-based HMS catalysts. To improve the adipic add yield, the influence of the transition metal as well as the effect of metal loading, reaction temperature and catalyst amount on the catalytic performances of Fe-HMS have been investigated in details. When Si/le atomic ratio - 100, Fe-HMS catalyst shows the highest activity, with a cyclohexanone conversion of 92.3% and adipic acid selectivity of 29.4%. The reaction pathway of cyclohexanone oxidation was further proposed based on experimental data. (C) 2020 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.