Studys On The New Technology Of Gas-liquid-solid Heterogeneous Catalytic Oxidation Of Ethylbenzene

The selective oxidation of hydrocarbons is of great importance and status in petroleum and chemistry industry.However,Ethylbenzene as an typical substituted aromatic hydrocarbons which has important scientific significance and application value.While because of high strengh and the C-H bond activation is difficult,lead to the condition of oxidation strict,energy consumption and low conversion rate;Meanwhile,the traditional oxidant most don't friendly to the environment.It is still a great challenge to discover catalyst system with high activity of selective oxidation of hydrocarbons under green oxidant(such as hydrogen peroxide or molecular oxygen).In this paper,we mainly design catalyst preparation;then,The liquid selective oxidation of ethylbenzene process route were studied which under atmospheric pressure and using hydrogen peroxide and O2 as the oxidant respectively.When use hydrogen peroxide as oxidant,the selective oxidation of ethylbenzene with acetyl acetone oxygen vanadium as catalyst were studied.The optimal reaction conditions under atmospheric pressure as follows:0.53g ethylbenzene and 0.013g VO(acac)2 were added into mixed solvent(3ml 2/3 mol/L H2SO4 and 7.5 mlacetonitrile),followed by adding 0.4ml 30%H2O2.Then the mixture was kept at 80 ? for 6h.The conversion of ethylbenzene and selectivity of acetophenone reached to 46.21%and 82.7%,respectively,and the effective utlization rate of H2O2 can reach 59.28%.When use oxygen as oxidant,the reaction under two kind of crafts conditions were studied separately,which taked nano-CuO and CuY molecular sieve as catalyst respectively for oxidation of ethylbenzene.(1)The CuO nanoparticles were synthesized using a solvothermal reaction between Copper acetate and ethanol.The structure of the CuO nanoparticles sample were characterized by XRD,FT-IR and TEM.CuO nanoparticles showed much higher activity in the liquid-phase aerobic oxidation of ethylbenzene with dioxygen under solvent-free condition.34.59%conversion of ethylbenzene with 97.9%selectivity for acetophenone(APO)and 1-phenyl ethanol(MPC)can be obtained under molecular oxygen at 110? for 24 h.The recovered catalyst could be reused without loss of activity.(2)When use CuY molecular sieve as catalyst,The conversion of ethylbenzene and selectivity of acetophenone reached to 24.18%and 75.2%,respectively,under the condition:10 mL ethylbenzene,0.1g catalyst,at 110? for 24 h.Moreover,we also investigated the effect of acetophenone,1-phenylethanol,benzaldehyde,styrene and water.The result show that only acetophenone can promote ethylbenzene oxidation reaction and other product have some inhibitory action in the reaction.