탄화수소에 의한 NO의 선택적 촉매 환원 반응에 대한 SnO<sub>2</sub>의 촉매 반응 연구

이오상; 이재도; 이순보; Ohsang Lee; Jae-Do Lee; Soon-Bo Lee

HWAHAK KONGHAK, Vol.38, No.5, 572-577, October, 2000

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탄화수소에 의한 NO의 선택적 촉매 환원 반응에 대한 SnO₂의 촉매 반응 연구

Selective Catalytic Reduction of NO with Hydrocarbons over SnO₂

이오상 ^†, 이재도, 이순보¹

한국화학연구소 화학소재연구부 4팀
¹성균관대학교 화학과

Ohsang Lee^†, Jae-Do Lee, and Soon-Bo Lee¹

Advanced Materials Division, Korea Research Institute of Chemical Technology, Korea
¹SungKyunKyuan University, Chemistry Department, Korea

E-mail:

초록

탄화수소가 공존하는 과잉 산소 분위기에서 SnO₂에 의하여 NO_x가 환원되는 반응 메커니즘과 환원 활성에 대하여 연구하였다. 승온탈착 실험에서 환원 처리된 SnO₂ 표면에 흡착된 NO는 150℃에서 NO로 탈착하고, 산화 처리된 경우에는 200, 300 및 390℃에서 NO₂로 탈착하는 것이 관찰되었다. 그러나 탄화수소(에틸렌, 프로필렌 및 프로판)를 이용한 선택적 촉매 환원 반응에서는 NO_x 환원 활성 온도 영역에서 오히려 NO₂의 배출이 억제되었다. 같은 실험조건에서 NO_x 환원 활성의 상대적 세기는 "에틸렌>프로필렌>>프로판"의 순으로 나타났으며, 본 실험 범위 내에서 반응 기체 중의 산소 농도 증가는 탄화수소 종류에 상관없이 NO_x 환원 활성을 감소시키는 것으로 나타났다. 또한 NO_x의 환원은 탄화수소의 연소와 함께 시작되는 것을 관찰할 수 있었다. 이러한 결과로부터, SnO₂에 의한 NO_x 환원은 SnO₂ 표면에 생성된 NO₂와 탄화수소 활성체에 의하여 이루어지는 것으로 해석하였다.

The mechanism and activity of SnO₂ for the selective catalytic reduction of NO_x at the atmosphere of hydrocarbons and an excess of oxygen has been studied. Temperature-programmed desorption showed that only NO was desorbed from the surface of reduced-SnO₂ at 150℃ and NO₂ was desorbed from the surface of oxidized-SnO₂ at 200, 300, and 390℃, respectively. For the selective catalytic reduction of NO_x by hydrocarbons(ethylene, propylene, and propane), however, the formation of NO₂ was depressed in the NO_x reduction temperature region. The relative intensities of NO_x reduction appeared to be the order of "ethylene>propylene>>propane" under the same experimental conditions. NO_x reduction activities had a tendency to decrease with increasing oxygen concentrations in the reaction gas compositions irrespective of hydrocarbon species our experimental conditions. It was observed that the NO_x reduction starts with the hydrocarbon combustion. From the results, it was proposed that NO_x was reduced by activated intermediate of hydrocarbons and NO₂ formed on SnO₂.

Keywords:SnO₂;Selective Catalytic Reduction;NO_x Catalyst

[References]

Iwamoto M, Yahiro H, Yu-u Y, Shundo S, Mizuni N, Shokubai, 32, 430 (1990)
Held W, Konig A, Richter T, Puppe L, SAE Paper, 900496 (1990)
Petunchi JO, Hall WK, Appl. Catal. B: Environ., 2, L17 (1993)
Inui T, Iwamoto M, Shimizu S, Proc. of 9th Congress on Catalysis, Budapest, B.8 (1992)
Hamada H, Kintaichi Y, Sasaki M, Ito T, Appl. Catal., 64, L1 (1990)
Kikuchi E, Yogo K, Tanaka S, Abe M, Chem. Lett., 1063 (1991)
Hamada H, Kintaichi Y, Sasaki M, Ito T, Tabata M, Appl. Catal., 70, L15 (1991)
Hosose H, Yahiro H, Mizuno N, Iwamoto M, Chem. Lett., 1859 (1991)
Hamada H, Kintaichi Y, Tabata M, Sasaki M, Ito T, Chem. Lett., 2179 (1991)
Cox DF, Fryberger TB, Semancik S, Phys. Rev., B, Condens. Matter, 38, 2072 (1988)
deFresart E, Draville J, Gilles JM, Appl. Surf. Sci., 11-12, 637 (1982)
Erickson JW, Semancik S, Surf. Sci., 187, L658 (1987)
Cox DF, Fryberger TB, Semancik S, J. Vac. Sci. Technol. A, 6, 828 (1988)
Cavicchi R, Tarlov M, Semancik S, J. Vac. Sci. Technol. A, 8, 2347 (1990)
Niwa M, Manami T, Kodama H, Hattori T, Murakami Y, J. Catal., 53, 198 (1978)
Takami J, Akiyama M, Xu C, Miura N, Yamazoe N, Shokubai, 31, 393 (1989)
Yamazoe N, Fuchigami J, Kishikawa M, Seiyama T, Surf. Sci., 86, 335 (1979)
Teraoka Y, Harada T, Iwasaki T, Ikeda T, Kagawa S, Chem. Lett., 773 (1993)
Yokoyama C, Misono M, J. Catal., 150(1), 9 (1994)
SPECRTA Instruments Inc., Technical Data, RGA Application Bulletin # 208

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[1] Iwamoto M, Yahiro H, Yu-u Y, Shundo S, Mizuni N, Shokubai, 32, 430 (1990)

[2] Held W, Konig A, Richter T, Puppe L, SAE Paper, 900496 (1990)

[3] Petunchi JO, Hall WK, Appl. Catal. B: Environ., 2, L17 (1993)

[4] Inui T, Iwamoto M, Shimizu S, Proc. of 9th Congress on Catalysis, Budapest, B.8 (1992)

[5] Hamada H, Kintaichi Y, Sasaki M, Ito T, Appl. Catal., 64, L1 (1990)

[6] Kikuchi E, Yogo K, Tanaka S, Abe M, Chem. Lett., 1063 (1991)

[7] Hamada H, Kintaichi Y, Sasaki M, Ito T, Tabata M, Appl. Catal., 70, L15 (1991)

[8] Hosose H, Yahiro H, Mizuno N, Iwamoto M, Chem. Lett., 1859 (1991)

[9] Hamada H, Kintaichi Y, Tabata M, Sasaki M, Ito T, Chem. Lett., 2179 (1991)

[10] Cox DF, Fryberger TB, Semancik S, Phys. Rev., B, Condens. Matter, 38, 2072 (1988)

[11] deFresart E, Draville J, Gilles JM, Appl. Surf. Sci., 11-12, 637 (1982)

[12] Erickson JW, Semancik S, Surf. Sci., 187, L658 (1987)

[13] Cox DF, Fryberger TB, Semancik S, J. Vac. Sci. Technol. A, 6, 828 (1988)

[14] Cavicchi R, Tarlov M, Semancik S, J. Vac. Sci. Technol. A, 8, 2347 (1990)

[15] Niwa M, Manami T, Kodama H, Hattori T, Murakami Y, J. Catal., 53, 198 (1978)

[16] Takami J, Akiyama M, Xu C, Miura N, Yamazoe N, Shokubai, 31, 393 (1989)

[17] Yamazoe N, Fuchigami J, Kishikawa M, Seiyama T, Surf. Sci., 86, 335 (1979)

[18] Teraoka Y, Harada T, Iwasaki T, Ikeda T, Kagawa S, Chem. Lett., 773 (1993)

[19] Yokoyama C, Misono M, J. Catal., 150(1), 9 (1994)

[20] SPECRTA Instruments Inc., Technical Data, RGA Application Bulletin # 208