ZrO2.SO42-에 담지된 백금촉매의 저온산화반응성에 대한 연구

김기석; 이태정; 김병삼; 김두성

Journal of the Korean Industrial and Engineering Chemistry, Vol.9, No.1, 141-148, February, 1998

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ZrO2.SO42-에 담지된 백금촉매의 저온산화반응성에 대한 연구

A Study on Low-Temperature Oxidation Reactivity of Pt/ZrO₂·SO₄^2- Catalyst

김기석, 이태정, 김병삼, 김두성

초록

초강산 담체인 ZrO₂·SO₄^2-에 담지된 백금촉매(0.2, 0.5wt% Pt)의 저온 산화반응성을 cyclohexane의 완전산화반응에 대하여 조사 하였다. 충전층 관형반응기에서 반응물질의 전화율로 측정된 촉매활성은 촉매의 산성도와 비표면적에 비례하여 증가하였다 Pt/ZrO₂·SO₄^2- 촉매 제조과정에서 K(potassium)를 첨가하여 촉매의 산성도와 비표면적을 감소시켰을 때 촉매활성은 K첨가량에 비례하여 감소하였다. 또한 Pt/ZrO₂·SO₄^2-촉매는 훨씬 더 큰 비표면적을 가진 Pt/SiO₂, 또는 Pt/Al₂O₃촉매보다 뛰어난 활성을 보였다 : l5,000ppm cyclohexane농도와 18,000hr^-1공간속도를 가진 반응물질 흐름을 250℃에서 0.2wt% Pt/ZrO₂·SO₄^2-촉매를 사용하여 전화시킨 결과 96%의 cyclohexane전화율을 보인 반면, 같은 반응조건 하에서 0.2wt% Pt/SiO₂와 0.2wt% Pt/Al₂O₃촉매는 각각 83%와 79%의 cyclohexane전화율을 보였다.

Reactivity of Pt catalysts(0.2, 0.5 wt% Pt) supported on solid super acid, ZrO₂·SO₄^2- for low-temperature oxidation was investigated for complete oxidation of cyclohexane. Catalytic activity measured as reactant conversion in a packed-bed tubular reactor increased in accordance with the acidity and specific surface area of the catalyst activity decreased in accordance with the amount of potassium added. In addition, Pt/ZrO₂·SO₄^2- catalyst exhibited an activity greater than that of a Pt/SiO₂ or Pt/Al₂O₃ catalyst possessing much larger specific surface area : at 250℃ for the reactant stream of 15.000 ppm cyclohexane concentration and 18,000 hr^-1 space velocity, a cyclohexane conversion as high as 96% was obtained over 0.2 wt% Pt/ZrO₂·SO₄^2-, whereas cyclohexane conversions over 0.2 wt% Pt/SiO₂ and 0.2 wt% Pt/A1₂O₃ were 83 and 79%, respectively.

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[1] Hino M, Kobayashi S, Arata K, J. Am. Chem. Soc., 101, 6439 (1979)

[2] Hino M, Arata K, J. Chem. Soc.-Chem. Commun., 851 (1980)

[3] Hino M, Arata K, Hyomen, 19, 75 (1981)

[4] Arata K, Hino M, Shokubai, 24, 241 (1982)

[5] Kayo A, Yamaguchi T, Tanabe K, J. Catal., 83, 99 (1983)

[6] Arata K, Adv. Catal., 37, 165 (1990)

[7] Srinivasan R, Keogh RA, Milburn DR, Davis BH, J. Catal., 153(1), 123 (1995)

[8] Olah GA, Prakash GKS, Sommer J, Science, 206, 13 (1979)

[9] Tabora JE, Davis RJ, J. Catal., 162(1), 125 (1996)

[10] Ishikawa A, Komai S, Satsuma A, Hattori T, Murakami Y, Appl. Catal. A: Gen., 110(1), 61 (1994)

[11] Keogh RA, Srinivasan R, Davis BH, Appl. Catal. A: Gen., 140(1), 47 (1996)

[12] Tanabe K, "Solid Acids and Bases," Academic Press, New York (1970)

[13] 이태정, 영남대학교 석사학위논문, 영남대학교 (1996)

[14] Corma A, Fornes V, Juanrajadell MI, Nieto JM, Appl. Catal. A: Gen., 116(1-2), 151 (1994)

[15] Comelli RA, Vera CR, Parera JM, J. Catal., 151(1), 96 (1995)

[16] Chen FR, Coudurier G, Joly JF, Vedrine JC, J. Catal., 143, 616 (1993)

[17] Morterra C, Cerrato G, Diciero S, Signoretto M, Pinna F, Strukul G, J. Catal., 165(2), 172 (1997)

[18] Kunimori K, Ikeda Y, Soma M, Uchijima T, J. Catal., 79, 185 (1973)

[19] Morterra C, Cerrato G, Bolis V, Catal. Today, 17, 505 (1993)

[20] Sparks DE, Keogh RA, Davis BH, Appl. Catal. A: Gen., 144(1-2), 205 (1996)

[21] Yaluris G, Larson RB, Kobe JM, Gonzalez MR, Fogash KB, Dumesic JA, J. Catal., 158(1), 336 (1996)

[22] Lopez T, Navarrete J, Gomez R, Novaro O, Figueras F, Armendariz H, Appl. Catal. A: Gen., 125(2), 217 (1995)