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은 촉매에 의한 에틸렌의 산화반응속도

Reaction Kinetics of Ethylene Oxidation on a Silver Catalyst

HWAHAK KONGHAK, April 1986, 24(2), 97-103(7), NONE
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Abstract

α-알루미나에 담지된 은 촉매를 합침법으로 제조하여 종래의 연구보다 넓은 반응물의 농도범위에 걸쳐서 에틸렌의 산화반응에 관한 실험연구를 수행하였다. 연속식 미분형 반응기를 사용하여 산화에틸렌과 이산화탄소의 생성반응속도를 측정함으로써 반응기구를 검증하고 각각의 반응속도식을 결정하였다.
각 반응의 반응속도식에 포함된 반응속도상수와 흡착평형상수를 온도의 함수로 나타내고, 이로부터 활성화에너지와 흡착열 및 흡착엔트로피를 구하였으며 이들 자료의 열역학적 의미를 고찰하여 반응기구의 타당성을 제시하였다.
연속식 적분형 반응기를 사용하여 실측한 각 성분의 접촉시간에 따른 분압분포곡선과 반응속도식을 적분하여 구한 분압분포곡선을 비교한 결과 반응물의 분압분포곡선들은 잘 부합하는 한편 생성물들에 대한 분포곡선들은 접촉시간이 증가함에 따라 점차 상위를 나타내는 것을 관찰하였다. 이는 접촉시간이 큰 경우에는 산화에틸렌의 완전산화반응이 무시될 수 없음을 암시하는 것으로 이해된다.
An experimental study has been conducted for the oxidation reaction of ethylene over a range of ethylene partial pressure wider than in the previous studies. The silver catalyst was prepared by the impregnation method with α-alumina as the support. A continuous flow reactor of differential type was employed to measure the reaction rate of ethylene oxide formation as well as that of carbon dioxide formation.
The reaction rate constants and the adsorption equilibrium constants were determined as functions of the temperature by applying the data to the rate expressions proposed.
These expressions then provided us with the activation energies, the enthalpies of adsorption, and the entropies of adsorption, the latter pair of which was tested to prove that the proposed reaction mechanism is thermodynamically meaningful.
The partial pressure profiles of the reactant and the products were measured from the integral flow reactor and compared with those obtained by integrating the reaction rate equations determined in this study. While the profiles for the reactant were in good agreement, those for the products tended to be discrepant as the contact time increased. This implies that the complete oxidation of ethylene oxide may have to be taken into consideration when the contact time is large.

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