MFI형 제올라이트 분리막을 이용한 에틸벤젠/파라자일렌 분리에 대한 연구

이기천; 전유권; 주영환; 최성환; 서영종; 설용건; Gi-cheon Lee; Yukwon Jeon; Young Hwan Chu; Seonghwan Choi; Young-Jong Seo; Yong-Gun Shul

Korean Chemical Engineering Research, Vol.51, No.4, 476-481, August, 2013

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MFI형 제올라이트 분리막을 이용한 에틸벤젠/파라자일렌 분리에 대한 연구

Ethylbenzene Separation from Ethylbenzene/p-xylene Mixture with MFI-type Zeolite Membranes

이기천, 전유권, 주영환^{1, †}, 최성환², 서영종², 설용건 ^†

연세대학교 화공생명공학과, 120-749 서울시 서대문구 연세로 50
¹상지대학교 신에너지자원공학과, 220-702 강원도 원주시 상지대길 83
²롯데케미칼(주), 305-726 대전시 유성구 장동 24-1

Gi-cheon Lee, Yukwon Jeon, Young Hwan Chu^{1, †}, Seonghwan Choi², Young-Jong Seo², and Yong-Gun Shul^†

Department of Chemical and Biomolecular Engineering, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 120-749, Korea
¹Department of New Energy, Resource Engineering, College of Science & Engineering, Sangji University, 83 Sangjidae-gil, Wonju-si, Gangwon 220-702, Korea
²The 4th Research Team, Daedeok Research Institute, Lotte Chemical Corp., Jang-dong #24-1, Yuseong-gu, Daejeon 305-726, Korea

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초록

본 연구에서는 물리적 특성이 유사한 에틸벤젠과 파라자일렌의 혼합물을 분리하고자 MFI형 제올라이트(TS-1, ZSM-5, Silicalite-1) 분리막을 제조하였으며 이를 이용하여 기상에서 분리 실험을 진행하였다. 제올라이트 입자가 코팅된 분리막을 제조함에 있어서 마이크로웨이브 합성 방법을 사용하여 합성 시간을 단축하였으며, 500 nm 내외의 균일한 입자를 튜브타입의 지지체 막에 안착시켜 제올라이트 입자가 3~4 μm두께로 치밀하게 코팅된 분리막을 제조하였다. 제조한 분리막으로 에틸벤젠/파라자일렌 혼합물 원료의 혼합비를 변경하여 투과 분리한 결과 에틸벤젠:파라자일렌=5:5 비율에서 가장 높은 분리도를 가짐을 알 수 있었다. 세 종류의 서로 다른 제올라이트 물질(TS-1, ZSM-5, Silicalite-1)을 각각 코팅하여 제조된 분리막을 이용하여 160~220 ℃의 실험온도에서 에틸벤젠/파라자일렌을 투과 실험을 실시한 결 과, TS-1 분리막이 1,666 mol/m2*s*Pa의 가장 높은 투과 플럭스를, Silicalite-1 분리막이 1.73의 가장 높은 분리도를 200 ℃의 온도에서 각각 보임을 확인할 수 있었다.

Ethylbenzene (EB) which has a similar physical properties with p-xylene (pX) was separated from EB/pX mixture by using MFI-type zeolite (TS-1, ZSM-5, and Silicalite-1) coated membranes. The zeolites were synthesized by microwave method to reduce the synthesis time and uniformly formed zeolite particles were coated on the α-almina tubular support with a thickness of 3-4 μm. Separation factor and permeation flux of the synthesized zeolite coated membranes were measured to survey the best performance of ethylbenzene separation from different composition of EB/pX mixtures. When the EB/pX mixture of 5:5 molar ratio applied for the separation experiment, it represented the highest separation factor. We also have studied about the effect of the atomic composition of zeolites on the separation performance within the temperature range from 160 to 220 ℃. TS-1 showed the highest permeation flux of 1,666 mol/m2*s*Pa and Silicate-1 showed the highest separation factor of 1.73 at 200 ℃ respectively.

Keywords:Ethylbenzene;p-xylene;Membrane;Zeolite;Microwave

[References]

Gu ZY, Jiang DQ, Wang HF, Cui XY, Yan XP, J.Phys. Chem. C., 114, 311 (2010)
Gu XH, Dong JH, Nenoff TM, Ozokwelu DE, J. Membr. Sci., 280(1-2), 624 (2006)
Lloyd B, Separation of Ethyl Benzene from p-xylene by Extractive Distillation, US Patent 5,425,855 (1994)
Tarditi AM, Irusta S, Lombardo EA, Chem. Eng. J., 122(3), 167 (2006)
Xomeritakis G, Tsapatsis M, Chem. Mater., 11, 875 (1999)
Lai ZP, Tsapatsis M, Nicolich JR, Adv. Funct. Mater., 14(7), 716 (2004)
Hu Y, Liu C, Zhang Y, Ren N, Tang Y, Microporous Mesoporous Mater., 119, 306 (2009)
Park SE, Chang JS, Hwang YK, Kim DS, Jhung SH, Hwang JS, Catal. Surv. Asia., 8, 91 (2004)
Baertsch CD, Funke HH, Falconer JL, Noble RD, J. Phys. Chem., 100(18), 7676 (1996)
Keizer K, Burggraaf AJ, Vroon ZAEP, Verweij H, J. Membr. Sci., 147(2), 159 (1998)
Lu YF, Ganguli R, Drewien CA, Anderson MT, Brinker CJ, Gong WL, Guo YX, Soyez H, Dunn B, Huang MH, Zink JI, Nature, 389(6649), 364 (1997)
Jeon YK, Lee GC, Chu YH, Choi SH, Seo YJ, Shul YG, Membrane Journal., 22, 120 (2012)
Jung KT, Shul YG, Chem. Mater., 9, 420 (1997)
Jung KT, Shul YG, J. Membr. Sci., 191(1-2), 189 (2001)
Taramasso M, Perego G, Notari B, “Preparation of Porous Crystalline Synthetic Material Comprised of Silicon and Titanium Oxides,” US Patent 4,410,501 (1983)
Sulikowski B, Rakoczy J, Hamdan H, Klinowski J, J. Chem. Soc., Chem. Commun., 1542 (1987)
Algieri C, Bernardo P, Golemme G, Barbieri G, Drioli E, J. Membr. Sci., 222(1-2), 181 (2003)
Xomeritakis G, Lai ZP, Tsapatsis M, Ind. Eng. Chem. Res., 40(2), 544 (2001)
Valerio G, Plevert J, Goursot A, di Renzo F, Phys. Chem. Chem. Phys., 2, 1091 (2000)

[Related Articles]

[1] Gu ZY, Jiang DQ, Wang HF, Cui XY, Yan XP, J.Phys. Chem. C., 114, 311 (2010)

[2] Gu XH, Dong JH, Nenoff TM, Ozokwelu DE, J. Membr. Sci., 280(1-2), 624 (2006)

[3] Lloyd B, Separation of Ethyl Benzene from p-xylene by Extractive Distillation, US Patent 5,425,855 (1994)

[4] Tarditi AM, Irusta S, Lombardo EA, Chem. Eng. J., 122(3), 167 (2006)

[5] Xomeritakis G, Tsapatsis M, Chem. Mater., 11, 875 (1999)

[6] Lai ZP, Tsapatsis M, Nicolich JR, Adv. Funct. Mater., 14(7), 716 (2004)

[7] Hu Y, Liu C, Zhang Y, Ren N, Tang Y, Microporous Mesoporous Mater., 119, 306 (2009)

[8] Park SE, Chang JS, Hwang YK, Kim DS, Jhung SH, Hwang JS, Catal. Surv. Asia., 8, 91 (2004)

[9] Baertsch CD, Funke HH, Falconer JL, Noble RD, J. Phys. Chem., 100(18), 7676 (1996)

[10] Keizer K, Burggraaf AJ, Vroon ZAEP, Verweij H, J. Membr. Sci., 147(2), 159 (1998)

[11] Lu YF, Ganguli R, Drewien CA, Anderson MT, Brinker CJ, Gong WL, Guo YX, Soyez H, Dunn B, Huang MH, Zink JI, Nature, 389(6649), 364 (1997)

[12] Jeon YK, Lee GC, Chu YH, Choi SH, Seo YJ, Shul YG, Membrane Journal., 22, 120 (2012)

[13] Jung KT, Shul YG, Chem. Mater., 9, 420 (1997)

[14] Jung KT, Shul YG, J. Membr. Sci., 191(1-2), 189 (2001)

[15] Taramasso M, Perego G, Notari B, “Preparation of Porous Crystalline Synthetic Material Comprised of Silicon and Titanium Oxides,” US Patent 4,410,501 (1983)

[16] Sulikowski B, Rakoczy J, Hamdan H, Klinowski J, J. Chem. Soc., Chem. Commun., 1542 (1987)

[17] Algieri C, Bernardo P, Golemme G, Barbieri G, Drioli E, J. Membr. Sci., 222(1-2), 181 (2003)

[18] Xomeritakis G, Lai ZP, Tsapatsis M, Ind. Eng. Chem. Res., 40(2), 544 (2001)

[19] Valerio G, Plevert J, Goursot A, di Renzo F, Phys. Chem. Chem. Phys., 2, 1091 (2000)