Pd 촉매상에서 일산화탄소 존재 하 수소의 선택적 산화반응: 담체 효과

김은정; 강동창; 신채호; Eun-Jeong Kim; Dong-Chang Kang; Chae-Ho Shin

Korean Chemical Engineering Research, Vol.55, No.1, 121-129, February, 2017

DOI10.9713/kcer.2017.55.1.121 Export Citation

Pd 촉매상에서 일산화탄소 존재 하 수소의 선택적 산화반응: 담체 효과

Selective Oxidation of Hydrogen Over Palladium Catalysts in the Presence of Carbon Monoxide: Effect of Supports

김은정, 강동창, 신채호^†

충북대학교 화학공학과, 28644 충청북도 청주시 서원구 충대로 1

Eun-Jeong Kim, Dong-Chang Kang, and Chae-Ho Shin^†

Department of Chemical Engineering, Chungbuk National University, 1, Chungdae-ro, Seowon-gu, Cheongju, Chungbuk, 28644, Korea

E-mail:

초록

TiO2, Al2O3, ZrO2, SiO2와 같은 다양한 담체에 습식함침법을 이용하여 Pd 기반 촉매를 제조하여 일산화탄소 존재하에 수소의 선택적 산화반응에 적용하였다. 제조된 촉매는 물리화학적 특성을 알아보기 위하여 XRD, N2 흡착, CO-, (CO+H2O)-TPD, CO-TPR, XPS등의 특성분석을 수행하였다. CO-TPD와 (CO+H2O)-TPD를 통해 CO2탈착에 대한 H2O의 영향을 알아보았으며 이러한 TPD 결과는 H2/CO 전환율과 상관관계가 있음을 확인하였다. 사용된 촉매 중에서 Pd/ZrO2 가 H2 전환율 측면에서 가장 활성이 좋은 것으로 나타났다. H2O가 첨가된 선택적 H2 산화반응에서는 H2O, CO, H2가 경쟁흡착을 하였으며, 첨가된 H2O가 CO 및 H2의 반응을 촉진시켰다.

Pd based catalysts were prepared by impregnating palladium precursor using incipient wetness method on TiO2, Al2O3, ZrO2, and SiO2 and were applied for the selective oxidation of H2 in the presence of CO. Their physicochemical properties were studied by X-ray diffraction (XRD), N2-sorption, temperature programmed desorption of CO (CO-TPD) and (CO+H2O)-TPD, temperature programmed reduction of CO (CO-TPR) and XPS a. The results of COand (CO+H2O)-TPD showed the correlation between peak temperature of TPD and catalytic activities for H2 and CO conversion. The Pd/ZrO2 catalyst exhibited the highest conversion of H2. The addition of H2O vapor promotes the conversion of H2 and CO by inducing easy desorption of CO and H2 in the competitive adsorption of H2O, CO and H2.

Keywords:Selective Oxidation;H2;CO;Palladium

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[4] Lim YI, Choi J, Moon HM, Kim GH, Korean Chem. Eng. Res., 54(3), 320 (2016)

[5] Osaki T, Narita N, Horiuchi T, Sugiyama T, Masuda H, Suzuki K, J. Mol. Catal. A-Chem., 125, 63 (1997)

[6] Wyse C, Vininski J, Watanabe T, Solid State Technol., 45, 125 (2002)

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[8] Pekridis G, Kalimeri K, Kaklidis N, Vakouftsi E, Iliopoulou EF, Athanasiou C, Marnellos GE, Catal. Today, 127(1-4), 337 (2007)

[9] Rostrupnielsen JR, Hansen JHB, J. Catal., 144, 38 (1993)

[10] Lu L, Li HZ, Hong YJ, Luo YF, Tang YW, Lu TH, J. Power Sources, 210, 154 (2012)

[11] Bulushev DA, Beloshapkin S, Ross JRH, Catal. Today, 154(1-2), 7 (2010)

[12] Banerjee R, Phan A, Wang B, Knobler C, Furukawa H, O'Keeffe M, Yaghi OM, Science, 319, 939 (2008)

[13] Lilga MA, Hallen RT, Nelson DA, J. Am. Chem. Soc., 33, 310 (1988)

[14] Tanaka KI, Shou M, He H, Shi XY, Catal. Lett., 110(3-4), 185 (2006)

[15] Shou M, Takekawa H, Ju DY, Hagiwara T, Lu DL, Tanaka K, Catal. Lett., 108(3-4), 119 (2006)

[16] Gorte RJ, Zhao S, Catal. Today, 104(1), 18 (2005)

[17] Moon DJ, Catal. Surv. Asia, 13, 191 (2009)

[18] Lee SH, Kim JN, Eom WH, Ryi SK, Park JS, Beak IH, Chem. Eng. J., 207-208, 521 (2012)

[19] Kochubey DI, Pavlova SN, Novgorodov BN, Kryukova GN, Sadykov VA, J. Catal., 161(2), 500 (1996)

[20] Bowker W, Stone P, Bennett R, Perkins N, Surf. Sci., 497, 155 (2002)

[21] Lee HH, Jang DH, Hong SC, Appl. Chem. Eng., 23(3), 253 (2012)

[22] Zhou RX, Zhao B, Yue BH, Appl. Surf. Sci., 254(15), 4701 (2008)

[23] Radkevich VZ, Senko TL, Wilson K, Grishenko LM, Zaderko AN, Diyuk VY, Appl. Catal. A: Gen., 335(2), 241 (2008)

[24] Park JH, Cho JH, Kim YJ, Kim ES, Han HS, Shin CH, Appl. Catal. B: Environ., 160-161, 135 (2014)