에틸렌 산화반응에 미치는 염소의 영향에 관한 속도록적 연구

박대원

HWAHAK KONGHAK, Vol.28, No.4, 373-378, August, 1990

Export Citation

에틸렌 산화반응에 미치는 염소의 영향에 관한 속도록적 연구

Kinetic Study on the Effect of Chlorine Promoter in Ethylene Epoxidation

박대원

초록

에틸렌의 산화에 의한 에틸렌오사이드의 제조반응에 미치는 염소의 영향을 고찰하기 위하여 염소를 처리한 촉매와 처리하지 않은 촉매에 대하여 속도론적 연구를 실시하였다. 촉매표면에 흡착된 염소는 반응의 활성을 감소시켰고 에틸렌옥사이드의 선택도를 증가시켰다. 염소처리된 촉매의 경우에도 Lang-muir-Hinshelwood 반응속도식을 적용할 수 있었고 촉매표면의 염소분율이 증가할수록 산소의 흡착평형 상수에 대한 에틸렌의 흡착평형 상수의 비(K_E/K_O)가 증가하였다. 한편 에틸렌옥사이드의 흡착에 의한 반응속도 억제현상은 에틸렌의 분압이 클수록 강하게 나타났으며 이와 같은 경향은 염소를 처리한 촉매의 경우에 더욱 현저하게 나타났다.

In order to investigate the effect of chlorine promoter on the epoxidation of ethylene to ethylene oxide, a steady state kinetic study was carried out with chlorinated and unchlorinated silver catalysts. Chlorine adsorbed on supported silver catalysts decreased overall activity and increased selectivity towards ethylene oxide. It was found that the Langmuir-Hinshelwood rate equation can be also applicable in the presence of chlorine promoter and the ratio of adsorption equilibrium constant of ethylene to that of oxygen (K_E/K_O)was increased with the increase of chlorine cov-erage. The decrease in the reaction rate caused by the adsorption of ethylene oxide was more enhanced with the in-crease of chlorine coverage and ethylene particle pressure in the reactant stream.

[References]

Sactler WMH, Backx C, van Santen RA, Catal. Rev.-Sci. Eng., 23, 127 (1981)
Verykios XE, Stern FP, Coughlin RW, Catal. Rev.-Sci. Eng., 22, 197 (1980)
Campbell CT, Paffett MT, Surf. Sci., 139, 396 (1984)
Boghosian S, Bebelis S, Vayenas CG, Papatheodorou GN, J. Catal., 117, 561 (1989)
Kilty PA, Sactler WMH, Catal. Rev.-Sci. Eng., 10, 1 (1974)
Cant NK, Hall WK, J. Catal., 52, 81 (1978)
Stoukides N, Vayenas CG, J. Catal., 69, 18 (1981)
Backx C, Moolhuysen J, Geenen P, vanSanten RA, J. Catal., 72, 364 (1981)
Grant RB, Lambert RM, J. Catal., 92, 364 (1985)
Force EL, Bell AT, J. Catal., 38, 440 (1975)
Campbell CT, J. Catal., 99, 28 (1986)
Tan SA, Grant RB, Lambert RM, J. Catal., 100, 383 (1986)
Campbell CT, Koel BE, J. Catal., 92, 272 (1985)
Ghalzali S, Park DW, Gau G, Appl. Catal., 6, 195 (1983)
Nelson GO, "Les Melanges de Gaz," Entr. Moderne d'Edition Tech. et Documentation, Paris (1973)
Park DW, Gau G, J. Catal., 105, 81 (1987)
Satterfield CN, "Heterogenous Catalysis in Practice," McGraw-Hill, New York, NY (1980)
Klugherz PD, Harriott P, AIChE J., 17, 856 (1971)
Park DW, Korean J. Chem. Eng., 7(1), 69 (1990)

[1] Sactler WMH, Backx C, van Santen RA, Catal. Rev.-Sci. Eng., 23, 127 (1981)

[2] Verykios XE, Stern FP, Coughlin RW, Catal. Rev.-Sci. Eng., 22, 197 (1980)

[3] Campbell CT, Paffett MT, Surf. Sci., 139, 396 (1984)

[4] Boghosian S, Bebelis S, Vayenas CG, Papatheodorou GN, J. Catal., 117, 561 (1989)

[5] Kilty PA, Sactler WMH, Catal. Rev.-Sci. Eng., 10, 1 (1974)

[6] Cant NK, Hall WK, J. Catal., 52, 81 (1978)

[7] Stoukides N, Vayenas CG, J. Catal., 69, 18 (1981)

[8] Backx C, Moolhuysen J, Geenen P, vanSanten RA, J. Catal., 72, 364 (1981)

[9] Grant RB, Lambert RM, J. Catal., 92, 364 (1985)

[10] Force EL, Bell AT, J. Catal., 38, 440 (1975)

[11] Campbell CT, J. Catal., 99, 28 (1986)

[12] Tan SA, Grant RB, Lambert RM, J. Catal., 100, 383 (1986)

[13] Campbell CT, Koel BE, J. Catal., 92, 272 (1985)

[14] Ghalzali S, Park DW, Gau G, Appl. Catal., 6, 195 (1983)

[15] Nelson GO, "Les Melanges de Gaz," Entr. Moderne d'Edition Tech. et Documentation, Paris (1973)

[16] Park DW, Gau G, J. Catal., 105, 81 (1987)

[17] Satterfield CN, "Heterogenous Catalysis in Practice," McGraw-Hill, New York, NY (1980)

[18] Klugherz PD, Harriott P, AIChE J., 17, 856 (1971)

[19] Park DW, Korean J. Chem. Eng., 7(1), 69 (1990)