FTIR을 이용한 Cu/SiO<SUB>2</SUB> 촉매상에서의 메타올 분해반응 연구

이동근; Bell AT

HWAHAK KONGHAK, Vol.34, No.3, 300-304, June, 1996

Export Citation

FTIR을 이용한 Cu/SiO₂ 촉매상에서의 메타올 분해반응 연구

FTIR Studies of Methanol Decomposition on Cu/SiO₂

이동근, Bell AT

초록

Cu/SiO₂촉매에서의 메탄올 분해반응을 연구하기 위하여 FTIR실험을 행하였다. 촉매 표면에 존재하는 메탄올 분해반응 중간물질로는 메탄올,methoxy, formaldehyde, methylenebis(oxy) 및 formate 그룹이 IR 실험결과 나타났으며, 구리의 표면상태가 이들 표면중간물질의 특성에 영향을 주었다. 환원된 촉매의 경우 methoxy가 매우 불안정하고 bidentate formate가 존재한 반면, 부분산화된 촉매의 경우 methoxy의 생성이 두드러졌고 unidentate formate가 존재하였다. 상온에서부터 300℃까지의 승온 FTIR스펙트럼 결과로부터 Cu/SiO₂ 촉매상에서의 메탄올 분해반응 메카니즘을 제시하였다.

Methanol decomposition on Cu/SiO₂has been investigated by means of Fourier transform infrared spectroscopy. Infrared spectroscopy experiments showed the following surface methanol decomposition intermediates on Cu/SiO₂ : methanol, methoxy,formaldehyde, methylenebis(oxy), and formate groups. The characteristics of surface intermediates were affected by the oxidation state of copper. On reduced copper methoxy was highly unstable and bidentate formate was formed, while on oxidized copper methoxy was stable and unidentate formate was formed. A mechanism of methanol decomposition was also proposed based on temperature programmed infrared experiment from 20 to 300℃.

Keywords:Methanol Decomposition;Cu/SiO₂;Formate;FTIR;Methoxy

[References]

Wachs IE, Madix RJ, J. Catal., 53, 208 (1978)
Sexton BA, Surf. Sci., 88, 299 (1979)
Sexton BA, Hughes AE, Auery NR, Appl. Surf. Sci., 22-23, 404 (1985)
Barmes C, Pudney T, Guo Q, Bowker M, J. Chem. Soc.-Faraday Trans., 86, 2693 (1990)
Ryberg R, Phys. Rev., B, Condens. Matter, 31, 2545 (1985)
Stohr J, Gland JL, Eberhath W, Outka D, Madis RJ, Sette F, Koestner RJ, Doebler C, Phys. Rev. Lett., 51, 2414 (1983)
Fu SS, Somorjai GA, J. Phys. Chem., 96, 4542 (1992)
Kohler MA, Lee JC, Trimm DL, Cant NW, Wainwright MS, Appl. Catal., 31, 309 (1987)
Evans JW, Wainwright MS, Waugh KC, Whan DA, J. Chem. Soc.-Faraday Trans., 2193 (1987)
Parris GE, Klier K, J. Catal., 97, 374 (1986)
Hicks RF, Kellner CS, Savatsky BJ, Hecker WC, Bell AT, J. Catal., 71, 216 (1981)
Sandoval MJ, M.S. Thesis, Dept. of Chem. Eng., U.C. Berkeley, CA (1993)
Berrello E, Zecchina A, Morterra C, J. Phys. Chem., 71, 2938 (1967)
Millar GJ, Rochester CH, Waugh KC, J. Chem. Soc.-Faraday Trans., 87, 2795 (1991)
Morrow BA, J. Chem. Soc.-Faraday Trans., 87, 2785 (1974)
Falk M, Whalley E, J. Chem. Phys., 34, 1554 (1961)
Millar GJ, Rochester CH, Waugh KC, J. Chem. Soc.-Faraday Trans., 87, 1491 (1991)
Millar GJ, Rochester CH, Howe C, Waugh KC, Mol. Phys., 76, 833 (1991)

[Referenced By]

[1] Wachs IE, Madix RJ, J. Catal., 53, 208 (1978)

[2] Sexton BA, Surf. Sci., 88, 299 (1979)

[3] Sexton BA, Hughes AE, Auery NR, Appl. Surf. Sci., 22-23, 404 (1985)

[4] Barmes C, Pudney T, Guo Q, Bowker M, J. Chem. Soc.-Faraday Trans., 86, 2693 (1990)

[5] Ryberg R, Phys. Rev., B, Condens. Matter, 31, 2545 (1985)

[6] Stohr J, Gland JL, Eberhath W, Outka D, Madis RJ, Sette F, Koestner RJ, Doebler C, Phys. Rev. Lett., 51, 2414 (1983)

[7] Fu SS, Somorjai GA, J. Phys. Chem., 96, 4542 (1992)

[8] Kohler MA, Lee JC, Trimm DL, Cant NW, Wainwright MS, Appl. Catal., 31, 309 (1987)

[9] Evans JW, Wainwright MS, Waugh KC, Whan DA, J. Chem. Soc.-Faraday Trans., 2193 (1987)

[10] Parris GE, Klier K, J. Catal., 97, 374 (1986)

[11] Hicks RF, Kellner CS, Savatsky BJ, Hecker WC, Bell AT, J. Catal., 71, 216 (1981)

[12] Sandoval MJ, M.S. Thesis, Dept. of Chem. Eng., U.C. Berkeley, CA (1993)

[13] Berrello E, Zecchina A, Morterra C, J. Phys. Chem., 71, 2938 (1967)

[14] Millar GJ, Rochester CH, Waugh KC, J. Chem. Soc.-Faraday Trans., 87, 2795 (1991)

[15] Morrow BA, J. Chem. Soc.-Faraday Trans., 87, 2785 (1974)

[16] Falk M, Whalley E, J. Chem. Phys., 34, 1554 (1961)

[17] Millar GJ, Rochester CH, Waugh KC, J. Chem. Soc.-Faraday Trans., 87, 1491 (1991)

[18] Millar GJ, Rochester CH, Howe C, Waugh KC, Mol. Phys., 76, 833 (1991)