|
Search / Korean Journal of Chemical Engineering
|
Korean Chemical Engineering Research, Vol.44, No.4, 387-392, 2006
카테콜의 선택적 합성을 위한 (Fe, Co)/Zeolites 촉매상에서 페놀의 수산화 반응
Hydroxylation of Phenol over (Fe, Co)/Zeolite Catalysts for the Selective Synthesis of Catechol
이온 교환법으로 (Fe, Co)/NaY, (Fe, Co)/NaBeta (Fe, Co)/HUSY 등 (Fe, Co)/zeolite 촉매를 제조하였으며, 카테콜을 합성하는 과산화수소에 의한 페놀의 수산화 반응에서 이들의 촉매 성능을 조사하였다. (Fe, Co)/NaBeta 촉매에서는 반응온도가 70 °C, 페놀/과산화수소(몰) 비가 3, 페놀/촉매(무게) 비가 50, 용매(물)/페놀(무게) 비가 6인 조건에서 페놀의 전환율은 22%, 수산화 반응에 대한 선택도는 77%, 카테콜에 대한 선택도는 70%, 카테콜/하이드로퀴논의 생성비는 2.5로 가장 좋은 반응 결과를 얻었다. (Fe, Co)/zeolite 촉매는 재생하여 반복 사용해도 성능이 저하되지 않았다. 반응 전후의 (Fe, Co)/zeolite 촉매를 XRD, UV-VIS DRS, XPS 등으로 조사하여, 이를 근거로 촉매 반응 결과를 해석하였다.
(Fe, Co)/zeolite catalysts such as (Fe, Co)/NaY, (Fe, Co)/NaBeta and (Fe, Co)/HUSY were prepared by ion-exchange method and their catalytic performance was examined in the hydroxylation of phenol with H2O2 for the production of catechol. The (Fe, Co)/NaBeta catalyst showed its best performance at reaction temperature=70 °C, molar ratio of phenol/H2O2=3, weight ratio of phenol/catalyst=50 and weight ratio of solvent (water)/phenol=6 as 20% of phenol conversion, 77% of the selectivity for the hydroxylation, 70% of the selectivity for catechol, and 2.5 of the formation ratio of catechol/hydroquinone. The (Fe, Co)/zeolite catalysts showed the reproducible activities without deactivation after repeated regeneration. The fresh and used(Fe, Co)/zeolites were characterized by XRD, UV-VIS DRS, and XPS and their catalytic performance was discussed based on these characterization results.
[References]
- Neta P, Fessenden RW, J. Phys. Chem., 78, 523, 1974
- Ogata Y, Urasaki I, Nagura K, Satomi N, Tetrahedron, 30(17), 3021, 1974
- Steenken S, O’Neill P, J. Phys. Chem., 81(6), 505, 1977
- Hamilton GA, Hamfin JW, Friedman JP, J. Am. Chem. Soc., 88(22), 5269, 1966
- Walling C, Johnson RA, J. Am. Chem. Soc., 97(2), 363, 1975
- Ai M, J. Catal., 54(2), 223, 1978
- Rakshe B, Ramaswamy V, Hegde SG, Vetrivel R, Ramaswamy AV, Catal. Lett., 45(1), 41, 1997
- Goldstein S, Czapski G, Rabani J, J. Phys. Chem., 98(26), 6586, 1994
- Zhu KZ, Liu CB, Ye XK, Wu Y, Appl. Catal. A: Gen., 168(2), 365, 1998
- Dubey A, Rives V, Kannan S, J. Mol. Catal. A-Chem., 181(2), 151, 2002
- Esposito A, Taramasso M, Neri C, “Hydroxylating Aromatic Hydrocarbons,” US Patent. No. 4,396,783, 1983
- Thangaraj A, Kumar R, Ratnasamy P, J. Catal., 131(1), 294, 1991
- Martens JA, Buskens P, Jacobs PA, van der Pol A, van Hooff JHC, Ferrini C, Kouwenhoven HW, Kooyman PJ, van Bekkum H, Appl. Catal. A: Gen., 99(1), 71, 1993
- Arends IWCE, Sheldon RA, Wallau M, Schuchardt U, Angew. Chem.-Int. Edit. Engl., 36(11), 1145, 1997
- Reddy JS, Sivasanker S, Ratnasamy P, J. Mol. Catal. A-Chem., 71(3), 373, 1992
- Camblor MA, Constantini M, Corma A, Esteve P, Gilbert L, Martinez A, Valencia S, Appl. Catal. A: Gen., 133(2), L185, 1995
- Wilkenhoner U, Langhendries G, van Laar F, Baron GV, Gammon DW, Jacobs PA, van Steen E, J. Catal., 203(1), 201, 2001
- Hari PR, Rao P, Ramaswamy AV, Appl. Catal. A: Gen., 93(2), 123, 1993
- Chou B, Tsai JL, Cheng S, Microporous Mesoporous Mater., 48(3), 309, 2001
- Awate SV, Waghmode SB, Patil KR, Agashe MS, Joshi PN, Korean J. Chem. Eng., 18(2), 257, 2001
- Lee CW, Ahn DH, Wang B, Hwang JS, Park SE, Microporous Mesoporous Mater., 44, 587, 2001
- Zhao W, Luo YF, Deng P, Li QZ, Catal. Lett., 73(2-4), 199, 2001
- Norena-Franco L, Hernandez-Perez I, Aguilar P, Maubert-Franco A, Catal. Today, 75(1-4), 189, 2002
- Wang L, Kong A, Chen B, Ding H, Shan Y, He M, J. Mol. Catal. A-Chem., 230(2), 143, 2005
- Xiao FS, Sun JM, Meng XJ, Yu RB, Yuan HM, Jiang DZ, Qiu SL, Xu RR, Appl. Catal. A: Gen., 207(1-2), 267, 2001
- Zhang H, Zhang X, Ding Y, Yan L, Ren T, Suo J, New J. Chem., 26(1), 376, 2002
- Jeong HC, Shim IW, Choi KY, Lee JK, Park JN, Lee CW, Korean J. Chem. Eng., 22(5), 657, 2005
- Yokoi T, Wu P, Tatsumi T, Catal. Commun., 4(1), 11, 2003
- Park JN, Wang J, Choi KY, Dong WY, Hong SI, Lee CW, J. Mol. Catal. A-Chem., 247(1), 73, 2006
- Wang J, Park JN, Wei XY, Lee CW, Chem. Commun., 5, 628, 2003
- Wang J, Park JN, Jeong HC, Choi KS, Wei XY, Hong SI, Lee CW, Energy Fuels, 18(2), 470, 2004
[Cited By]
- Kwon SY, Yoon S, Kim H, Lee JW, Lee CW, Korean Chemical Engineering Research, 48(4), 423, 2010
- Yoon S, Kwon SY, Lee CW, Korean Journal of Chemical Engineering, 28(1), 71, 2011
- Kwon SY, Yoon SH, Lee JM, Chang JS, Lee CW, Korean Chemical Engineering Research, 49(2), 151, 2011
|