이산화탄소의 수소화반응에 의한 메탄올 합성

이희준; 박진우; 함현식

HWAHAK KONGHAK, Vol.34, No.6, 716-720, December, 1996

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이산화탄소의 수소화반응에 의한 메탄올 합성

Methanol Synthesis by the Hydrogenation of Carbon Dioxide

이희준, 박진우, 함현식

초록

Cu/MgO, Cu/ZnO, Cu/ZnO/Al₂O₃ 및 Au/TiO₂와 Cu/ZnO/Al₂O₃연합촉매 상에서 이산화탄소의 수소화반응에 의하여 메탄올을 합성하였다. 반응조건은 160-250℃, H₂/CO₂=3 및 25bar였으며 고정층 반응기를 이용하였다. 본 연구에서 사용한 촉매중 Cu/ZnO/Al₂O₃가 최고로 활성이 좋았다. Au/TiO₂와 Cu/ZnO/Al₂O₃촉매를 series로 연결하여 실험한 결과 Cu/ZnO/Al₂O₃촉매만 사용한 경우보다 약 16% 정도의 메탄올 선택도 향상을 얻을 수 있었다. Cu/ZnO/Al₂O₃촉매의 반응 전 . 후 XRD실험을 통해서 본 촉매계의 활성점으로 알려져 있는 Cu⁺ site는 발견할 수 없었고 다만 Cu는 금속상태로만 관찰되었다.

Methanol synthesis through the hydrogenation of CO₂ was investigated over Cu/MgO, Cu/ZnO, Cu/ZnO/Al₂O₃, and Cu/ZnO/Al₂O₃ combined with Au/TiO₂ catalysts at 160-250℃, H₂/ CO₂=3, 25bar, and in packed-bed reactor. Among the catalysts used, Cu/ZnO/Al₂O₃showed the highest catalytic activity. The combination of Au/TiO₂ and Cu/ZnO/Al₂O₃ catalysts in series increased the methanol selectivity to about 16%. With the XRD result, Cu⁺ site which has been known as an active site of the Cu/ZnO/Al₂O₃catalyst system was not observed, whereas only XRD peak for Cu was observed.

Keywords:Carbon Dioxide Hydrogenation;Methanol Synthesis;Copper/Zirconia/Alumina;Catalyst Characterization(XRD)

[References]

Galvin D, Bower C, Proc. of the 1st JAPAN-EC, 96 (1991)
Gushee DE, Chemtech., 470 (1989)
Lee JS, Catalysis, 7(1), 26 (1991)
MacDongll LV, Catal. Today, 8, 337 (1991)
Wade LE, Gengelbach RB, Trumbley JL, Hallbauer WL, Kirk-Othmer Encyclopedia of Chemical Technology, 3rd ed., Wiley-Interscience, New York, 15, 398 (1981)
Sakurai H, Tsubota S, Haruta M, Appl. Catal., 102, 125 (1993)
Inoue T, Iizuke T, Tanabe K, Bull. Chem. Soc. Jpn., 60, 2663 (1987)
Stiles AB, "Catalyst Manufacture," Dekker, 127 (1983)
Stout GH, Jensen LH, "X-ray Sturcture Determination," New York (1968)
Frohlich C, Koppel RA, Baiker A, Appl. Catal., 106, 275 (1993)
Cheng WH, Kung HH, "Methanol Production and Use," Dekker, New York, 51 (1994)
Leach BE, 2, 215 (1983)
Gillies MT, "C₂-Based Chemicals from Hydrogen and Carbon Monoxide," Noyes Data Corporation, New Jersey, 200 (1982)
Bartley GJJ, Burch R, Appl. Catal., 43, 141 (1988)
Herman RG, Klier K, Simmons GW, Finn BP, Bulko JB, Kobylinski J, J. Catal., 56, 407 (1979)

[Referenced By]

[1] Galvin D, Bower C, Proc. of the 1st JAPAN-EC, 96 (1991)

[2] Gushee DE, Chemtech., 470 (1989)

[3] Lee JS, Catalysis, 7(1), 26 (1991)

[4] MacDongll LV, Catal. Today, 8, 337 (1991)

[5] Wade LE, Gengelbach RB, Trumbley JL, Hallbauer WL, Kirk-Othmer Encyclopedia of Chemical Technology, 3rd ed., Wiley-Interscience, New York, 15, 398 (1981)

[6] Sakurai H, Tsubota S, Haruta M, Appl. Catal., 102, 125 (1993)

[7] Inoue T, Iizuke T, Tanabe K, Bull. Chem. Soc. Jpn., 60, 2663 (1987)

[8] Stiles AB, "Catalyst Manufacture," Dekker, 127 (1983)

[9] Stout GH, Jensen LH, "X-ray Sturcture Determination," New York (1968)

[10] Frohlich C, Koppel RA, Baiker A, Appl. Catal., 106, 275 (1993)

[11] Cheng WH, Kung HH, "Methanol Production and Use," Dekker, New York, 51 (1994)

[12] Leach BE, 2, 215 (1983)

[13] Gillies MT, "C₂-Based Chemicals from Hydrogen and Carbon Monoxide," Noyes Data Corporation, New Jersey, 200 (1982)

[14] Bartley GJJ, Burch R, Appl. Catal., 43, 141 (1988)

[15] Herman RG, Klier K, Simmons GW, Finn BP, Bulko JB, Kobylinski J, J. Catal., 56, 407 (1979)