摘要
在高压间歇釜式反应器中,考察了6种催化剂对三氯氢硅(TCS)歧化反应的催化效果.选取催化效果最佳的大孔弱碱性阴离子交换树脂PA100为催化剂,研究了催化剂用量、颗粒尺寸、温度和反应时间对三氯氢硅歧化反应的影响,并通过测定不同反应条件下三氯化硅转化率随时间的变化,获得三氯氢硅歧化反应的动力学模型.结果表明,在催化剂用量为0.133,4,gcat/gTCS、温度为343.15,K的条件下PA100的催化活性最好.获得的动力学模型表明,三氯氢硅歧化反应为二级反应,正反应的指前因子和活化能分别为5.292,m3/(kmol·s)和38.498,k J/mol,逆反应的指前因子和活化能分别为4.779,m3/(kmol·s)和27.387,k J/mol.在实验条件范围内对获得的动力学方程进行了验证,误差小于5%,表明模型具有较好的拟合精度,能准确反映三氯氢硅歧化反应过程及其动力学特征.
The redistribution reaction of trichlorosilane(TCS) was studied by using six different kinds of catalyst in a high pressure batch reactor.The catalytic activity of the macroporous weakly basic anion acid exchange resin PA100 is the best, so PA100 was selected as the catalyst. Effects of catalyst quantity,particle size, operating temperature and reaction time were examined. The reaction kinetic parameters were obtained by measuring the change of trichlorosilane conversion with reaction time. It has been found that the best condition for the conversion of trichlorosilane is at 343.15 K with a mass dosage of 0.133 4 gcat/g TCS by using PA100 as the catalyst. The kinetic data analysis suggests that the redistribution reaction of trichlorosilane is second order for the forward reaction and the backward reaction. The pre-exponential factor and activation energy are 5.292 m3/(kmol·s) and 38.498 k J/mol for the forward reaction, and the pre-exponential factor and activation energy are 4.779 m3/(kmol·s) and 27.387 k J/mol for the backward reaction.Comparing the calculated values obtained by using the obtained kinetic equation with the experimental values, the margin of error is less than 5%. The results indicate that the model exhibits high fitting precision for simulation, which can well reflect the reaction process and kinetics of the redistribution reaction of trichlorosilane.
出处
《天津大学学报(自然科学与工程技术版)》
EI
CAS
CSCD
北大核心
2015年第10期908-913,共6页
Journal of Tianjin University:Science and Technology
关键词
三氯氢硅
歧化反应
催化剂
动力学
trichlorosilane
redistribution reaction
catalyst
kinetics