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Received October 5, 2007
Accepted October 18, 2007
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Titanium Silicalite-1 촉매를 이용한 Allylchloride 에폭시화 반응: 속도론적 고찰
A Kinetic Study of Allylchloride Epoxidation using Titanium Silicalite-1 Catalyst
인하대학교 화학공학과, 402-751 인천시 남구 용현동 253 1한화석유화학(주) 중앙연구소, 305-804 대전시 유성구 신성동 6
Department of Chemical Engineering, Inha University, 253 Yonghyun-dong, Nam-gu, Incheon 402-751, Korea 1R&D Center, Hanwha Chemical, 6 Shinsung-dong, Yusung-gu, Daejon 305-804, Korea
whasahn@inha.ac.kr
Korean Chemical Engineering Research, February 2008, 46(1), 142-146(5), NONE Epub 28 February 2008
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Abstract
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.
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