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Hydrogen, oxygen as raw materials, direct synthesis of hydrogen peroxide in line with the concept of atom economy, is the ideal hydrogen peroxide production methods; low temperature, hydrogen peroxide as the oxidant, the TS-1 zeolite catalytic ammonia oxidation of cyclohexanone with high activity and high selectivity characteristics. The integration of the above two reaction processes, is feasible; theory also has a very attractive to reduce the complexity of the process, to improve the utilization of raw materials, to reduce energy consumption. Based on this, direct synthesis of hydrogen, oxygen, hydrogen peroxide and its study with the integration process of the ammoxidation reaction of cyclohexanone. Using impregnation prepared a series of transition metal-modified M-Pd/TS-1 (M = Ce, La, Pt, Fe, Co, Ni, Cr, Mn, Zn, Cd, Cu) catalyst, and The catalyst prepared is used under atmospheric pressure of hydrogen, the the oxygen direct synthesis reaction of hydrogen peroxide. The results show that the the M select Ce, the highest yield of the aimed product of hydrogen peroxide. Examine the nO2/nH2 than the gas flow rate, reaction time and reaction conditions on the H2 conversion, H2O2 selectivity and yield. Relatively optimum conditions, ie nO2/nH2 ratio of 3, the gas flow rate of 25 mL · min-1, the reaction time of 3 h, the the H2O2 yield of up to 25.7%, 18.7 mol · mol-TOF value 1 · h-1, H2O2 quality solution percentage was 0.8%, compared with the experimental results reported under atmospheric pressure have a higher level of Establish the appropriate conditions of ammonia oxidation reaction of cyclohexanone, including the ratio of ammonia / ketone, the reaction temperature, amount of catalyst, etc., and the effects of the hydrogen peroxide concentration, solvent methanol ammoxidation reaction of cyclohexanone. Within a certain range, the With dropwise addition used the decrease of the hydrogen peroxide concentration, the yield of cyclohexanone oxime. In addition, for the ammoxidation reaction of cyclohexanone, in methanol as solvent, the yield of cyclohexanone oxime will be significantly reduced. -Step integration method and two-step integration method, respectively direct synthesis of hydrogen and oxygen through the integration of the ammonia oxidation reaction of hydrogen peroxide and cyclohexanone. Step integration method, the methanol / water solvent, hydrogen, oxygen, first for 3 h, n (cyclohexanone) / n (ammonia) than the ingredient ratio of 2.5:2, put into the ring in the reactor cyclohexanone ammonia oxidation raw material, and then for 3 h, the yield of cyclohexanone oxime was 4.8%. In a two-step integration method, the methanol / water solvent hydroxide, direct synthesis of hydrogen peroxide used in ammonia oxidation reaction of cyclohexanone, the first step hydrogen peroxide in a yield of 14.1%, the second step in the n ( cyclohexanone) / n (ammonia) ratio of 2.5:2 of the cases, the hydrogen peroxide utilization is 9.6%, cyclohexanone oxime in a yield of 5.8%, in general, hydrogen, in a yield of 1.3% ; when using water as a solvent, the hydroxide obtained by the direct synthesis of hydrogen peroxide used in the subsequent cyclohexanone ammonia oxidation reaction, the first step through the hydrogen peroxide in a yield of 7.2%, the second step, the use of hydrogen peroxide rate of 24.9%, the cyclohexanone oxime yield of 14.9% overall, 1.8% of the yield of hydrogen.
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