浆态床二甲醚合成的本征动力学研究

在温度240～282℃、压力4～6MPa、x0H2/x0CO=0 99～2 33、相对甲醇催化剂进气空速为10000h-1、甲醇合成催化剂4g、甲醇脱水催化剂0 05～0 30g的反应条件下,于250mL高压搅拌釜中进行了浆态床二甲醚合成过程的本征动力学研究。在消除了内外扩散传质影响和保持催化剂稳定性的前提下,测定了本征动力学数据。采用Graaf的甲醇合成动力学模型和Bercic的甲醇脱水动力学模型对实验数据进行拟合后,甲醇、二甲醚和CO2的表观生成速率的计算值和实验值误差分别在±13%,±15%和±26%以内。

Study on Intrinsic Kinetics of Dimethyl Ether Synthesis in Slurry Reactor

Kinetics of dimethyl ether (DME) synthesis from syngas on commercial copper-based methanol catalyst and γ-alumina dehydration catalyst suspended in liquid paraffin was studied.A 250 mL agitating slurry reactor was used.The reaction conditions were p=4.0～6.0 MPa,t=240～282 ℃,x~0_(H_2)/x~0_(CO)=0.99～2.33,GHSV=10 000 h~(-1),4 g of methanol catalyst and 0.05～0.3 g of methanol dehydration catalyst.Under steady state,kinetic experimental data were measured after preconditioning that both inner-particle and intra-particle diffusion were not rate control steps in overall reaction-mass transfer process.Kinetic models based on methanol synthesis model proposed by Graaf and methanol dehydration model by Bercic were adopted for fitting experimental data.In parameter estimation,deviations between experimental and calculated values of methanol,dimethyl ether and carbon dioxide apparent formation rates were respectively less than ±13%,±15% and (±26%) respectively.