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Received April 23, 2010
Accepted May 12, 2010
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수소생산을 위한 메탄 부분산화용 코발트와 니켈촉매의 반응특성 연구
Partial Oxidation of Methane for Hydrogen Production over Co and Ni Catalysts
창원대학교 화공시스템공학과, 641-773 경남 창원시 사림동 9번지
Department of Chemical Engineering, Changwon National University, 9 Sarim-dong, Changwon-si, Gyeongnam 641-773, Korea
jdhan@changwon.ac.kr
Korean Chemical Engineering Research, December 2010, 48(6), 776-783(8), NONE Epub 11 January 2011
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Abstract
수소생산을 위한 메탄의 부분산화용 촉매로 알루미나에 담지된 코발트와 니켈 촉매를 함침법으로 제조하였다. 메탄의 부분산화반응을 위한 이들 촉매의 반응활성은1기압, CH4/O2=2.0과 450~650 ℃의 온도영역에서 조사하였다. 담지량이 다른 코발트촉매와 니켈촉매의 반응활성을 비교하고 코발트촉매에 니켈을 첨가한 이성분금속 촉매의 반응활성을 조사하였다. 그리고 코발트촉매와 니켈촉매에 첨가된 Ce와 La의 첨가효과를 조사하였다. 이들 촉매의 특성은 XRD와 SEM/EDX로 분석하였다. 코발트와 니켈은 10 wt%의 담지량이 적절한 것으로 나타났다. 이들 10 wt% 담지 코발트와 니켈촉매는 열역학적 평형값에 가까운 메탄의 전환율과 CO의 선택성을 나타내었으나 H2의 선택성은 평형값보다 다소 낮게 나타났다. 코발트촉매에 니켈을 첨가한 이성분금속 촉매에서 H2의 선택성은 증가하였으나 전환율을 고려하면 니켈을 첨가한 이점은 나타나지 않았다. 코발트촉매에서는 Ce의 첨가와 니켈촉매에서는La의 첨가로 메탄의 전환율과 수소의 선택성을 높일 수 있었다.
Co and Ni catalysts supported on Al2O3 for partial oxidation of methane producing hydrogen were synthesized using impregnation to incipient wetness. The activities of these catalysts for the partial oxidation of methane was investigated at 1 atm and CH4/O2=2.0 in the temperature range of 450~650 ℃. The reaction activity of Ni/Al2O3 and Co/Al2O3 catalysts with different loading was investigated. And the beneficial effects of Ni addition to Co/Al2O3 and the promotional effects of Ce and La addition to Ni/Al2O3 and Co/Al2O3 were investigated. These catalysts were_x000D_
characterized by XRD and SEM/EDX. Comparing catalyst loadings, 10 wt% Co and 10 wt% Ni were found to be optimal at the experimental conditions. The 10 wt% Ni/Al2O3 and 10 wt% Co/Al2O3 catalysts in partial oxidation of methane showed CH4 conversions and CO selectivity close to the thermodynamic equilibrium levels, but showed lower H2 selectivity than equilibrium level. The addition of Ni to Co/Al2O3 exhibited higher H2 selectivity but beneficial effect was not observed in the CH4 conversion. Addition of Ce to Co/Al2O3 and addition of La to Ni/Al2O3 improved the CH4 conversion level and H2 selectivity.
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Enger BC, Lodeng R, Holmen A, Appl. Catal. A: Gen., 346(1-2), 1 (2008)
Ayabe S, Omoto H, Utaka T, Kikuchi R, Sasaki K, Teraoka Y, Eguchi K, Appl. Catal. A: Gen., 241(1-2), 261 (2003)
Newson E, Truong TB, Int. J. Hydrog. Energy., 28, 1379 (2003)
Hu YH, Ruckenstein E, Adv. Catal., 48, 297 (2004)
Choudhary VR, Sansare SD, Mamman AS, Appl. Catal. A: Gen., 90, L1 (1992)
Wang M, Weng W, Zheng H, Yi X, Huang C, Wan H, J. Nat. Gas. Chem., 18, 300 (2009)
Kim SB, Kim YK, Lim YS, Kim MS, Hahm HS, Korean J. Chem. Eng., 20(6), 1023 (2003)
Kim SB, Shin KS, Park ES, Kwak YC, Cheon HJ, Hahm HS, HWAHAK KONGHAK, 41(1), 20 (2003)
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Tsang SC, Claridge JB, Green ML, Catal. Today, 23(1), 3 (1995)
Slagtern A, Swaan HM, Olsbye U, Dahl IM, Mirodatos C, Catal. Today, 46(2-3), 107 (1998)
Lodeng R, Bjorgum E, Enger BC, Eilertsen JL, Holmen A, Krogh B, Ronnekleiv M, Rytter E, Appl. Catal. A: Gen., 333(1), 11 (2007)
Kim KH, Lee SY, Nam SW, Lim TH, Hong SA, Yoon KJ, Korean J. Chem. Eng., 23(1), 17 (2006)
Dissanayake D, Rosynek MP, Kharas KCC, Lunsford JH, J. Catal., 132, 117 (1991)
Christensen KO, Chen D, Lodeng R, Holmen A, Appl. Catal. A: Gen., 314(1), 9 (2006)
Sun WZ, Jin GQ, Guo XY, Catal. Commun., 6, 135 (2005)
Choudhary VR, Rane VH, Rajput AM, Appl. Catal. A: Gen., 162(1-2), 235 (1997)
Zhu TL, Flytzani-Stephanopoulos M, Appl. Catal. A: Gen., 208(1-2), 403 (2001)
Enger BC, Lodeng R, Holmen A, J. Catal., 262(2), 188 (2009)
Rogatis LD, Montini T, Cognigni A, Olivi L, Fornasiero P, Catal. Today, 145, 176 (2009)
Gao XX, Huang CJ, Zhang NW, Li JH, Weng WZ, Wan HL, Catal. Today, 131(1-4), 211 (2008)
Requies J, Barrio VL, Cambra JF, Guemez MB, Arias PL, Parola VL, Pena MA, Fierro JLG, Fuel, 87, 3223 (2008)
Enger BC, Lodeng R, Holmen A, Appl. Catal. A: Gen., 364(1-2), 15 (2009)
Liu ZW, Jun KW, Roh HS, Park SE, Oh YS, Korean J. Chem. Eng., 19(5), 735 (2002)
Torniainen PM, Chu X, Schmidt LD, J. Catal., 146(1), 1 (1994)
Woo SW, Kang Y, Kang KS, Kim CH, Kim CS, Park CS, Korean Chem. Eng. Res., 46(6), 1113 (2008)
Swaan HM, Rouanet R, Widyananda P, Mirodatos C, Stud. Surf. Sci. Catal., 107, 447 (1997)
Enger BC, Lødeng R, Holmen A, J. Catal., 262(2), Issue 2, 10 March 2009, Pages 188-198 (2009)
Cao L, Chen Y, Li W, Stud. Surf. Sci. Catal., 107, 467 (1997)
Ma D, Mei D, Li X, Gong M, Chen Y, J. Rare. Earths., 24, 451 (2006)
