이성분계 Nb/Fe 혼합산화물 촉매에 의한 아황산가스의 제거

정종국; 이석희; 박대원; 우희철; Jong Kook Chung; Seok Hee Lee; Dae Won Park; Hee Chul Woo

Clean Technology, Vol.12, No.2, 87-94, June, 2006

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이성분계 Nb/Fe 혼합산화물 촉매에 의한 아황산가스의 제거

Removal of SO2 over Binary Nb/Fe Mixed Oxide Catalysts

정종국, 이석희 , 박대원 ¹, 우희철 ^†

부경대학교 응용화학공학부, 608-739 부산시 남구 용당동 산 100
¹부산대학교 화학공학과, 609-735 부산시 금정구 장전동 산 30번지

Jong Kook Chung, Seok Hee Lee , Dae Won Park¹, and Hee Chul Woo^†

Faculty of Applied Chemical Engineering, Pukyong University, San 100, Yongdang-dong, Nam-gu,Busan 608-739, Korea
¹Department of Chemical Engineering, Pusan University, San 30, Jangjeon-dong, Geumjeong-gu,Busan 609-735, Korea

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초록

철과 니오븀의 몰비가 1/0, 10/1, 5/1, 1/1, 1/5, 1/10 및 0/1 인 철-니오븀 촉매상에서 일산화탄소에 의한 아황산가스의 원소 황으로의 환원이 고정층 흐름반응기에서 연구되었다. 촉매 활성 및 선택도 면에서 우수한 상승효과를 철-니오븀 촉매에서 관찰할 수 있었으며, 가장 우수한 촉매 현상은 철과 니오븀의 몰비 1/1 촉매에서 관찰되었다. 활성화된 철-니오븀 촉매의 활성상은 XRD와 XPS 의 분석결과 FeS2 로 확인되었다. 일산화탄소에 의한 아황산가스의 선택적 환원은 카르보닐 황화물 반응중간체 메커니즘을 따르는 것으로 나타났다.

The reduction of SO2 to elemental sulfur by CO over a series of iron niobate with nominal Nb/Fe atomic ratios of 1/0, 10/1, 5/1, 1/1, 1/5, 1/10 and 0/1 was studied with a flow fixed-bed reactor. Strong synergistic phenomena in catalytic activity and selectivity were observed for the iron niobate catalysts, and the best catalytic performance was observed for the catalyst with Fe/Nb atomic ratio of 1/1. The active phase of the activated iron niobate catalysts was identified to be FeS2 using XRD and XPS. Selective reduction of SO2 by CO was followed by the COS intermediate mechanism.

Keywords:Nb/Fe mixed oxide;XRD;XPS;Carbon monoxide;Sulfur dioxide;Selective reduction;COS intermediate mechanism

[References]

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Pieplu A, Saur O, Lavalley JC, Legendre O, Nedez C, Catal. Rev.-Sci. Eng., 40(4), 409 (1998)
Khalafalla SE, Foerster EF, Hass LA, Ind. Eng. Chem. Prod. Res. Dev., 10, 133 (1971)
Khalafalla SE, Foerster EF, Hass LA, J. Catal., 24, 121 (1972)
Ma JX, Fang M, Lau NT, Appl. Catal. A: Gen., 150(2), 253 (1997)
Liu W, Sarofim AF, Flytzanistephanopoulos M, Appl. Catal. B: Environ., 4(2-3), 167 (1994)
Paik SC, Kim H, Chung JS, Catal. Today, 38(2), 193 (1997)
Zhaoliang Z, Jun M, Xiyao Y, J. Mol. Catal. A-Chem., 195, 189 (2003)
Tanabe K, Catal. Today, 8, 1 (1990)
Vedrine JC, Coudurier G, Ouqour A, Deoliveira PG, Volta JC, Catal. Today, 28(1-2), 3 (1996)
Wachs IE, Jehng JM, Deo G, Hu H, Arora N, Catal. Today, 28(1-2), 199 (1996)
Tanabe K, Okazaki S, Appl. Catal. A: Gen., 133(2), 191 (1995)
Paulis M, Martin M, Soria DB, Diaz A, Odriozola JA, Montes M, Appl. Catal. A: Gen., 180(1-2), 411 (1999)
Pittman RM, Bell AT, Catal. Lett., 24(1-2), 1 (1994)
Penners NHG, Koopal LK, Colloids Surf., 19, 337 (1986)
JCPDS database (Fe2O3 : 72-0469, Nb2O5 : 07-0061, FeNbO4 : 70-2275, FeS2 : 71-2219)
Gnanasekar KI, Jayaraman V, Prabhu E, Gnanasekaran T, Periaswami G, Sens. Actuators B-Chem., 55, 170 (1999)
Noda Y, Shimada M, Koizumi M, Kanamaru F, J. Solid State Chem., 28, 379 (1979)
Schmidbauer E, Schneider J, J. Solid State Chem., 134, 253 (1997)
Moulder JF, Stickle WF, Sobol PE, Bomben KD, “Handbook of X-ray photoelectron spectroscopy,” Phys. Electron., INC (1995)
Bukhtiyarova GA, Bukhtiyarov VI, Sakaeva NS, Kaichev VV, Zolotovskii BP, J. Molec. Catal. A-Chem., 158, 251 (2000)

[Related Articles]

[1] 홍지형, “유해 대기오염 물질의 국내 배출 실태,” 한국공업화학회, 제 4회 환경기술심포지움, 89 (2000)

[2] Pieplu A, Saur O, Lavalley JC, Legendre O, Nedez C, Catal. Rev.-Sci. Eng., 40(4), 409 (1998)

[3] Khalafalla SE, Foerster EF, Hass LA, Ind. Eng. Chem. Prod. Res. Dev., 10, 133 (1971)

[4] Khalafalla SE, Foerster EF, Hass LA, J. Catal., 24, 121 (1972)

[5] Ma JX, Fang M, Lau NT, Appl. Catal. A: Gen., 150(2), 253 (1997)

[6] Liu W, Sarofim AF, Flytzanistephanopoulos M, Appl. Catal. B: Environ., 4(2-3), 167 (1994)

[7] Paik SC, Kim H, Chung JS, Catal. Today, 38(2), 193 (1997)

[8] Zhaoliang Z, Jun M, Xiyao Y, J. Mol. Catal. A-Chem., 195, 189 (2003)

[9] Tanabe K, Catal. Today, 8, 1 (1990)

[10] Vedrine JC, Coudurier G, Ouqour A, Deoliveira PG, Volta JC, Catal. Today, 28(1-2), 3 (1996)

[11] Wachs IE, Jehng JM, Deo G, Hu H, Arora N, Catal. Today, 28(1-2), 199 (1996)

[12] Tanabe K, Okazaki S, Appl. Catal. A: Gen., 133(2), 191 (1995)

[13] Paulis M, Martin M, Soria DB, Diaz A, Odriozola JA, Montes M, Appl. Catal. A: Gen., 180(1-2), 411 (1999)

[14] Pittman RM, Bell AT, Catal. Lett., 24(1-2), 1 (1994)

[15] Penners NHG, Koopal LK, Colloids Surf., 19, 337 (1986)

[16] JCPDS database (Fe2O3 : 72-0469, Nb2O5 : 07-0061, FeNbO4 : 70-2275, FeS2 : 71-2219)

[17] Gnanasekar KI, Jayaraman V, Prabhu E, Gnanasekaran T, Periaswami G, Sens. Actuators B-Chem., 55, 170 (1999)

[18] Noda Y, Shimada M, Koizumi M, Kanamaru F, J. Solid State Chem., 28, 379 (1979)

[19] Schmidbauer E, Schneider J, J. Solid State Chem., 134, 253 (1997)

[20] Moulder JF, Stickle WF, Sobol PE, Bomben KD, “Handbook of X-ray photoelectron spectroscopy,” Phys. Electron., INC (1995)

[21] Bukhtiyarova GA, Bukhtiyarov VI, Sakaeva NS, Kaichev VV, Zolotovskii BP, J. Molec. Catal. A-Chem., 158, 251 (2000)