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        Selective hydrogenation of benzene over Ru supported on surface modified TiO2

        Fang Hao,Jingsong Zheng,Donghong Ouyang,Wei Xiong,Pingle Liu,Hean Luo 한국화학공학회 2021 Korean Journal of Chemical Engineering Vol.38 No.4

        A series of catalysts with ruthenium nanoparticles (NPs) loaded on the binary oxide TS (TiO2-SiO2) support were prepared by facile sol-gel method for benzene selective hydrogenation. Different mole ratios of Ti/Si were investigated. The catalytic structure, composition, hydrophilicity, electronic state and acidity were characterized. The results indicate that the acidity of the samples increases gradually with the increase of the SiO2 amount. The dispersion of ruthenium nanoparticles was improved on binary oxide support compared with TiO2 and an obvious Ru size effect appeared with the increase of Ti/Si molar ratio. It was also found that the hydrophilicity of the supports could be efficiently improved by introducing a small amount of SiO2 to TiO2, which may be due to the large amount of surface hydroxyl groups on the binary oxide samples after SiO2 introduction. This result was consistent with the increasing trend of cyclohexene yield, indicating that the surface hydroxyl groups play a significant role in the motivation of cyclohexene desorption. Ru/TS (7 : 1) showed the best catalytic performance of 38.2% yield to cyclohexene with the highest initial selectivity to cyclohexene (S0) of 87.3%. The catalytic stability experiments showed that the yield of cyclohexene could maintain at 30% after five cycles.

      • KCI등재

        Nitrogen-doped graphene loaded non-noble Co catalysts for liquid-phase cyclohexane oxidation with molecular oxygen

        Fang Hao,Yuan Sun,Yidi Wang,Yang Lv,Pingle Liu,Xiong Wei,Hean Luo 한국화학공학회 2021 Korean Journal of Chemical Engineering Vol.38 No.8

        Selective aerobic oxidation of cyclohexane to cyclohexanone and cyclohexanol (KA oil) with high yield under mild and green conditions is still a significant challenge in the current chemical industry. Herein, nitrogen doped graphene loaded non-noble Co (Co-N-rGO) catalysts, prepared by a facile post-impregnation method, exhibited a high catalytic performance and stability in liquid phase cyclohexane oxidation with molecular oxygen. The experiment and characterization results show that N doping in the catalysts promotes Co metal particle dispersion and induces carbon film coating on Co to prevent leaching and agglomeration. Besides, density functional theory (DFT) calculations show that N doping is beneficial to the O-O bonds breaking in cyclohexyl-hydroperoxides (CHHP), thereby promoting the dissociation of CHHP and enhancing the yield to KA oil. In addition, the catalyst can be easily separated without appreciable loss of catalytic activity after recycling for five times, and show potential industrial application value for the catalytic oxidation of cyclohexane to KA oil in the chemical industry.

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