Catalysis Today, Vol.248, 91-100, 2015
Effect of low hydrogen to palladium molar ratios in the direct synthesis of H2O2 in water in a trickle bed reactor
Application of a trickle bed reactor (TBR) renders a very compact solution to carry out direct synthesis of hydrogen peroxide in water over a carbon supported palladium. The laboratory scale reactor was filled with silica particles (50-70 mesh) physically mixed with 37.5 to 75 mg of 5%Pd/C particles. The reaction conditions applied were 15 degrees C, 15-28 barg, 0.5 to 6 mL min(-1) of liquid and 4.0-4.5 mL min(-1) of gas flowrate (86.7/11/2.23 mol% of CO2/O-2/H-2). Thus, we demonstrated that the ratio between H-2 and Pd is one of the key factors to achieve optimized, higher yields of hydrogen peroxide. Consequently, low H-2 concentrations lead to low productivities. One of the least studied parameters, addressed here, is the ratio between the bed filling (SiO2) and the catalyst; i.e. the active catalytic species dilution effect. In short, it was found that when the amount of Pd was reduced below 0.094 mg Pd cm(-3) SiO2 the highest productivity of H2O2 could be achieved. The selectivity obtained were between 5.3 and 38.0%, respectively, corresponding to turn-over-frequencies (TOF) ranging from 65 to 921 mmol H2O2 gPd(-1) h(-1). (C) 2014 Elsevier B.V. All rights reserved.
Keywords:Hydrogen peroxide;Direct synthesis;Heterogeneous catalysis;Palladium on carbon;Gas solubility;Trickle bed reactor