수열 합성법과 마이크로파 가열법으로 제조한 TS-1 촉매에 의한 페놀 수산화 반응: 용매의 영향

권송이; 윤성훈; 이종민; 장종산; 이철위; Song-Yi Kwon; SongHun Yoon; Jong-Min Lee; Jong-San Chang; Chul Wee Lee

Korean Chemical Engineering Research, Vol.49, No.2, 151-154, April, 2011

Export Citation

수열 합성법과 마이크로파 가열법으로 제조한 TS-1 촉매에 의한 페놀 수산화 반응: 용매의 영향

Phenol Hydroxylation over TS-1 Synthesized by Hydrothermal and Microwave Heating Method: Solvent Dependence

권송이, 윤성훈 , 이종민, 장종산 , 이철위 ^†

한국화학연구원 그린화학연구단, 305-600 대전광역시 유성구 장동 100

Song-Yi Kwon, SongHun Yoon , Jong-Min Lee, Jong-San Chang , and Chul Wee Lee^†

Green Chemistry Division, KRICT, 100 Jang-dong, Yuseong-gu, Daejeon 305-600, Korea

E-mail:

초록

수열 합성법과 마이크로파 가열법으로 제조한 TS-1의 촉매 성능 평가를 과산화수소수를 이용한 페놀 수산화 반응에서 수행하였는데 아세톤과 메탄올 및 물의 세 가지 용매를 사용하여 각 용매에서의 페놀 전환율과 생성물의 선택도 변화를 관찰하였다. 수열 합성법으로 제조한 TS-1과 마이크로파 가열법으로 합성한 TS-1의 XRD, EDS, SEM, BET 흡착/탈착 시험을 통해 촉매의 특성을 비교·분석하였고 마이크로파 가열법으로 합성한 TS-1이 수열 합성으로 제조한 TS-1과 상이한 페놀 전환율과 생성물의 선택도를 보이는 이유에 대해서 설명하였다.

Catalytic activity such as conversion and selectivity on the phenol hydroxylation over TS-1 prepared by hydrothermal method and microwave heating method, respectively, was compared and discussed for understanding the dependence of solvent such as water, methanol, acetone, respectively, during phenol hydroxylation, with hydrogen peroxide. Basic physical properties such as XRD, EDS, SEM and N2 adsorption/desorption were determined and compared. The relationship between catalytic activity and physical properties of TS-1 was explained.

Keywords:TS-1;Hydrothermal;Microwave Heating;Phenol Hydroxylation;Solvent Effect

[References]

Clerici MG, Bellussi G, Romano U, J. Catal., “Synthesis of Propylene Oxide from Propylene and Hydrogen Peroxide Catalyzed by Titanium Silicalite.", 129(1), 159 (1991)
Taramasso M, Perego G, Notari B, “Preparation of Porous Crystalline Synthetic Material Comprised of Silicon and Titanium Oxides,” U.S. Patent, No. 4,410,501 (1983)
Kannan S, Dubey A, Knozinger H, J. Catal., “Synthesis and Characterization of CuMgAl Ternary Hydrotalcites as Catalysts for the Hydroxylation of Phenol.", 231(2), 381 (2005)
Ahn WS, Lee KY, Catal. Surv. Asia., “Extensions in the Synthesis and Catalytic Application of Titanium Silicalite-1.", 9(1), 51 (2005)
Xu CH, Jin TH, Jhung SH, Chang JS, Hwang JS, Park SE, Catal. Today, “Hydrophobicity and Catalytic Properties of Ti-MFI Zeolites Synthesized by Microwave and Conventional Heating.", 111(3-4), 366 (2006)
Weitkamp J, Ernst S, Roland E, Thiele GF, “The Modified Hydrophobicity Index as a Novel Method for Characterizing the Surface Properties of Titanium Silicalites,” Zeolite, 763-770 (1997)
Corma A, Esteve P, Martinez A, J. Catal., “Solvent Effects During the Oxidation of Olefins and Alcohols with Hydrogen Peroxide on Ti-Beta Catalyst: the Influence of the Hydrophilicity-hydrophobicity of the Zeolite.", 161(1), 11 (1996)
Thangaraj A, Kumar R, Mirajkar SP, Ratnasamy P, J. Catal., “Catalytic Properties of Crystalline Titanium Silicalites; I. Synthesis And Characterization of Titanium-rich Zeolites with MFI Structure.", 130(1), 1 (1991)
Park JN, Shin CH, Baeg JO, Lee CW, Korean Chem. Eng. Res., “Hydroxylation of Phenol over (Fe, Co)/zeolite Catalysts for the Selective Synthesis of Catechol.", 44(4), 387 (2006)
Serrano DP, Sanz R, Pizarro P, Moreno I, de Frutos P, Blazquez S, Catal. Today., “Preparation of Extruded Catalysts Based on TS-1 Zeolite for Their Application in Propylene Epoxidation,”, 143(1-2), 151 (2009)
Hwang YK, Chang JS, Park SE, Kim DS, Kwon YU, Jhung SH, Hwang JS, Park MS, Angew. Chem. Int. Ed., “Microwave Fabrication of MFI Zeolite Crystals with a Fibrous Morphology and Their Applications.", 117(4), 556 (2005)
Wilkenhoner U, Langhendries G, van Laar F, Baron GV, Gammon DW, Jacobs PA, van Steen E, J. Catal., “Influence of Pore and Crystal Size of Crystalline Titanosilicates on Phenol Hydroxylation in Different Solvent.", 203(1), 201 (2001)
Thangaraj A, Puthoor L, Sivasanker S, Indian. J. Chem., “Solvent Effects in the Hydroxylation of Phenol with H2O2 over TS-1,”, 33A, 255 (1994)
Thangaraj A, Kumar R, Mirajkar SP, Ratnasamy P, J. Catal., “Catalytic Properties of Crystalline Titanium Silicalites. II. Hydroxylation of Phenol with Hydrogen Peroxide over TS-1 Zeolites.", 131(1), 294 (1991)

[Related Articles]

[1] Clerici MG, Bellussi G, Romano U, J. Catal., “Synthesis of Propylene Oxide from Propylene and Hydrogen Peroxide Catalyzed by Titanium Silicalite.", 129(1), 159 (1991)

[2] Taramasso M, Perego G, Notari B, “Preparation of Porous Crystalline Synthetic Material Comprised of Silicon and Titanium Oxides,” U.S. Patent, No. 4,410,501 (1983)

[3] Kannan S, Dubey A, Knozinger H, J. Catal., “Synthesis and Characterization of CuMgAl Ternary Hydrotalcites as Catalysts for the Hydroxylation of Phenol.", 231(2), 381 (2005)

[4] Ahn WS, Lee KY, Catal. Surv. Asia., “Extensions in the Synthesis and Catalytic Application of Titanium Silicalite-1.", 9(1), 51 (2005)

[5] Xu CH, Jin TH, Jhung SH, Chang JS, Hwang JS, Park SE, Catal. Today, “Hydrophobicity and Catalytic Properties of Ti-MFI Zeolites Synthesized by Microwave and Conventional Heating.", 111(3-4), 366 (2006)

[6] Weitkamp J, Ernst S, Roland E, Thiele GF, “The Modified Hydrophobicity Index as a Novel Method for Characterizing the Surface Properties of Titanium Silicalites,” Zeolite, 763-770 (1997)

[7] Corma A, Esteve P, Martinez A, J. Catal., “Solvent Effects During the Oxidation of Olefins and Alcohols with Hydrogen Peroxide on Ti-Beta Catalyst: the Influence of the Hydrophilicity-hydrophobicity of the Zeolite.", 161(1), 11 (1996)

[8] Thangaraj A, Kumar R, Mirajkar SP, Ratnasamy P, J. Catal., “Catalytic Properties of Crystalline Titanium Silicalites; I. Synthesis And Characterization of Titanium-rich Zeolites with MFI Structure.", 130(1), 1 (1991)

[9] Park JN, Shin CH, Baeg JO, Lee CW, Korean Chem. Eng. Res., “Hydroxylation of Phenol over (Fe, Co)/zeolite Catalysts for the Selective Synthesis of Catechol.", 44(4), 387 (2006)

[10] Serrano DP, Sanz R, Pizarro P, Moreno I, de Frutos P, Blazquez S, Catal. Today., “Preparation of Extruded Catalysts Based on TS-1 Zeolite for Their Application in Propylene Epoxidation,”, 143(1-2), 151 (2009)

[11] Hwang YK, Chang JS, Park SE, Kim DS, Kwon YU, Jhung SH, Hwang JS, Park MS, Angew. Chem. Int. Ed., “Microwave Fabrication of MFI Zeolite Crystals with a Fibrous Morphology and Their Applications.", 117(4), 556 (2005)

[12] Wilkenhoner U, Langhendries G, van Laar F, Baron GV, Gammon DW, Jacobs PA, van Steen E, J. Catal., “Influence of Pore and Crystal Size of Crystalline Titanosilicates on Phenol Hydroxylation in Different Solvent.", 203(1), 201 (2001)

[13] Thangaraj A, Puthoor L, Sivasanker S, Indian. J. Chem., “Solvent Effects in the Hydroxylation of Phenol with H2O2 over TS-1,”, 33A, 255 (1994)

[14] Thangaraj A, Kumar R, Mirajkar SP, Ratnasamy P, J. Catal., “Catalytic Properties of Crystalline Titanium Silicalites. II. Hydroxylation of Phenol with Hydrogen Peroxide over TS-1 Zeolites.", 131(1), 294 (1991)