Ni-Mo/γ-Al2O3 촉매를 사용한 1,1,2-trichloroethane의 수첨탈연소 반응에서 전처리 조건과 첨가된 Ni의 영향

최영헌; 이화영; Young Heon Choi; Wha Young Lee

Journal of the Korean Industrial and Engineering Chemistry, Vol.11, No.6, 687-692, October, 2000

Effect of Pretreatment Condition and Added Ni on Catalyst Performance of Ni-Mo/γ-Al2O3 Catalysts in the Hydrodechlorination of 1,1,2-trichloroethane

최영헌, 이화영 ^†

서울대학교 공과대학 응용화학부, 서울 151-742

Young Heon Choi, and Wha Young Lee^†

Division of Chemical Engineering, Seoul National University, Shilim-dong, Kwanak-ku, Seoul 151-742, Korea

E-mail:

초록

수소화 촉매인 Ni-Mo/γ-Al2O3를 이용하여 이염화에탄 제조공정의 주요 부산물인 1,1,2-삼염화에탄을 에틸렌으로 변환시키기 위한 기상 수첨탈염소 반응을 상압, 300 ℃에서 수행하였다. 촉매 제조시 주요 변수로 작용하는 소성온도, Ni의 함량 및 촉매의 전처리 조건에 따른 반응성을 조사하였다. 황전처리된 Ni-Mo/γ-Al2O3는 MoS2 활성점에 의해 높은 활성을 나타냄을 확인하였다. Ni의 함량이 증가함에 따라 전환율과 선택도가 증가하였으며, 첨가된 Ni은 주촉매로서 독립된 활성을 나타내었다. 소성 온도가 400-450 ℃ 범위에서 에틸렌 수율이 가장 좋았으며, 반응 중에 발생한 HCl은 촉매 비활성화의 주된 요인이었다.

The gas phase hydrodechlorination of 1,1,2-trichloroethane (TCEA), which is a major chlorinated organic waste produced in the EDC (Ethylene dichloride) process was carried out to form ethylene over Ni-Mo/γ-Al2O3 catalysts at 300 ℃ and atmospheric pressure. The effects of calcination temperature, Ni loading and pretreatment conditions on catalyst performance of Ni-Mo/-Al2O3 were investigated. Sulfidation of Ni-Mo/γ-Al2O3 showed high activity at the active site of MoS2. Conversion and ethylene selectivity increased with the Ni loading, and ethylene yield exhibited the maximum at a calcination temperature of 450 ℃. The added Ni played an important role in the hydrodechlorination of TCEA. The HCl decreased catalytic activity and hydrogenation ability of catalysts.

Keywords:1,1,2-trichloroethane (TCEA);Ni-Mo/γ-Al2O3;Calcination temperature;Ni;HCl

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Choi YH, Lee WY, Catal. Lett., accepted (2000)
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[Related Articles]

[1] Cisneros MD, Rougue B, U.S. Patent, 5,430,215 (1995)

[2] Harley JD, Holbrook MT, Smith D, Cisneros MD, U.S. Patent, 5,453,557 (1995)

[3] Ito LN, Jones ME, Bare SR, U.S. Patent, 5,637,548 (1997)

[4] Stach J, Pekarek V, Endrst R, Hetflejs J, Chemosphere, 39, 2391 (1999)

[5] Coute N, Ortego JD, Richardson JT, Twigg MV, Appl. Catal. B: Environ., 19(3-4), 175 (1998)

[6] Trillas M, Peral J, Domenech X, J. Chem. Technol. Biotechnol., 67(3), 237 (1996)

[7] Gampine A, Eyman DP, J. Catal., 179(1), 315 (1998)

[8] Coq B, J. Mol. Catal., 71, 317 (1992)

[9] Coq B, Ferret G, J. Catal., 101, 434 (1986)

[10] Takita Y, Tamaha H, Hashida M, Ishihara T, Chem. Lett., 715 (1990)

[11] Kuznetsova NN, Lokteva ES, Lunin VV, Yudina SL, J. Catal., 131, 412 (1991)

[12] Lapierre RB, Wu D, Weiss AH, J. Catal., 52, 59 (1978)

[13] Getty EE, Petrosius SC, Drago RS, J. Mol. Catal., 67, 127 (1991)

[14] Suzdorf AR, Morozov SV, Anshits NN, Tsiganova SI, Anshits AG, Catal. Lett., 29(1-2), 49 (1994)

[15] Choi YH, Lee WY, Catal. Lett., accepted (2000)

[16] Kim DI, Allen DT, Ind. Eng. Chem. Res., 36(8), 3019 (1997)

[17] Park YC, Ph.D. Dissertation, Seoul National University, Seoul, Korea (1996)

[18] Dufresene PP, Grimblot J, Bonnelle JP, J. Phys. Chem., 85, 2344 (1985)

[19] Richardson JT, Ind. Eng. Chem. Fundam., 3, 154 (1964)

[20] Yang SH, Satterfield CN, J. Catal., 81, 168 (1983)

[21] Yang SH, Satterfield CN, Ind. Eng. Chem., 23, 20 (1984)

[22] Coq B, Cognion JM, Figueras F, Tournigant D, J. Catal., 141, 21 (1993)

[23] Tavoularis G, Keane MA, J. Mol. Catal. A-Chem., 142, 187 (1999)