Korean Chemical Engineering Research, Vol.46, No.1, 142-146, February, 2008
Titanium Silicalite-1 촉매를 이용한 Allylchloride 에폭시화 반응: 속도론적 고찰
A Kinetic Study of Allylchloride Epoxidation using Titanium Silicalite-1 Catalyst
E-mail:
초록
Titanium silicalite-1 촉매를 175 ℃에서 2일간 SiO2-TiO2 xerogel을 전구체로 사용하여 수열 합성하였고, 이를 이용하여 allylchloride(ALC) 에폭시화 반응의 속도론 인자를 도출하기 위해 반응온도 25~55 ℃, ALC의 농도 0.2~3.0M, 과산화수소의 농도 0.2~1.5M 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.
Titanium silicalite-1 catalyst was prepared using a SiO2-TiO2 xerogel and applied to allylchloride (ALC) epoxidation by H2O2 as oxidant in a batch reactor. The reaction temperature was varied from 25 to 55 ℃, and the concentrations of ALC and H2O2 were changed from 0.2 to 3 M and from 0.2 to 1.5M, 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 H2O2 and ALC were determined to be 0.41 and 0.52, respectively.
- Taramasso M, Perego G, Notari B, U.S. Patent No. 4, 410, 501 (1983)
- Notari B, Adv. Catal., 41, 253 (1996)
- Vayssilov GN, Catal. Rev. Sci. Eng., 39(3), 209 (1997)
- Gao HX, Lu GX, Sue JH, Li SB, Appl. Catal. A: Gen., 138(1), 27 (1996)
- Tomoyuki K, Yasuo K, Stud. Surf. Sci. Catal., 121, 355 (1998)
- Shetti VN, Srinivas D, Ratnasamy P, J. Mol. Catal. A-Chem., 210(1-2), 171 (2004)
- Wroblewska A, J. Mol. Catal. A-Chem., 229(1-2), 207 (2005)
- Wang QF, Mi ZT, Wang YQ, Wang L, J. Mol. Catal. A-Chem., 229(1-2), 71 (2005)
- Serrano DP, Garcia RA, Otero D, Moreno I, Stud. Surf. Sci. Catal., 158, 477 (2005)
- Uguina MA, Serrano DP, Ovejero G, Vangrieken R, Camacho M, Appl. Catal. A: Gen., 124(2), 391 (1995)
- Kim WJ, Kim TJ, Ahn WS, Lee YJ, Yoon KB, Catal. Lett., 91(1-2), 123 (2003)
- Ban HJ, Lee KY, Lee JK, Chung ST, Ahn WS, Korean Chem. Eng. Res., 44(2), 121 (2006)
- Ahn WS, Lee KY, Catal. Surv. Asia, 9, 51 (2005)