A Kinetic Study of Allylchloride Epoxidation using Titanium Silicalite-1 Catalyst

Titanium Silicalite-1 촉매를 이용한 Allylchloride 에폭시화 반응: 속도론적 고찰

  • 양승태 (인하대학교 화학공학과) ;
  • 최정식 (인하대학교 화학공학과) ;
  • 권영철 (한화석유화학(주) 중앙연구소) ;
  • 이상욱 (한화석유화학(주) 중앙연구소) ;
  • 안화승 (인하대학교 화학공학과)
  • Received : 2007.10.05
  • Accepted : 2007.10.18
  • Published : 2008.02.28

Abstract

Titanium silicalite-1 catalyst was prepared using a $SiO_2-TiO_2$ xerogel and applied to allylchloride (ALC) epoxidation by $H_2O_2$ as oxidant in a batch reactor. The reaction temperature was varied from 25 to $55^{\circ}C$, and the concentrations of ALC and $H_2O_2$ were changed from 0.2 to 3 M and from 0.2 to 1.5 M, respectively. The kinetic data obtained were applied to the power rate law, Eley-Rideal, and a Langmuir-Hinshelwood model, and power rate law fits the experimental data best. Activation energy was 27.9 kJ/mol, and the reaction orders with respect to $H_2O_2$ and ALC were determined to be 0.41 and 0.52, respectively.

Titanium silicalite-1 촉매를 $175^{\circ}C$에서 2일간 $SiO_2-TiO_2$ xerogel을 전구체로 사용하여 수열 합성하였고, 이를 이용하여 allylchloride(ALC) 에폭시화 반응의 속도론 인자를 도출하기 위해 반응온도 $25{\sim}55^{\circ}C$, ALC의 농도 0.2~3.0 M, 과산화수소의 농도 0.2~1.5 M 영역에서 촉매 반응실험을 수행하였다. 초기농도법을 이용하여 반응속도를 구한 후, power rate law, Eley-Rideal, 및 Langmuir-Hinshelwood 모델에 적용한 결과, 큰 차이는 없으나 power rate law에서 실험치와 예측치가 가장 우수하게 일치하였고, 이때 활성화 에너지는 29.7 kJ/mol, 과산화수소에 대한 반응차수는 0.41, ALC에 대한 반응차수는 0.52였다.

Keywords

Acknowledgement

Supported by : 한화석유화학(주) 중앙연구소

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