Transactions of the Korean hydrogen and new energy society (한국수소및신에너지학회논문집)

The Korean Hydrogen and New Energy Society (한국수소및신에너지학회)
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A Study on the Characteristics of Ni/Ce0.9Gd0.1O2-x and Cu/Ce0.9Gd0.1O2-x Catalysts for Methanol Steam Reforming Synthesized by Solution Combustion Process

용액연소법으로 합성한 Ni/Ce0.9Gd0.1O2-x와 Cu/Ce0.9Gd0.1O2-x 촉매의 메탄올 수증기 개질 특성 연구

  • LEE, JUNGHUN (The 4th R&D institute, Agency for Defense Development)
  • 이정훈 (국방과학연구소 제4기술연구본부)
  • Received : 2019.02.25
  • Accepted : 2019.06.30
  • Published : 2019.06.30
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Abstract

Methanol is a liquid fuel which could also be produced from renewable energy sources and has appreciably high energy density. In this work, we investigated the application of $Ce_{0.9}Gd_{0.1}O_{2-x}$ supported Cu and Ni catalysts for hydrogen production via methanol steam reforming. Catalysts were synthesized by solution combustion synthesis. The prepared catalysts with various active materials and Cu loading amounts were tested in a reactor at $200-300^{\circ}C$, 0-5 barg range and steam to methanol molar ratio was 1.5. The catalytic properties of Cu and Ni were compared, and the catalytic performance was shown to depend on the amounts of metal loading and operating conditions such as reaction temperature and pressure.

Keywords

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Fig. 1. Experimental set-up for methanol steam reforming

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Fig. 2. SEM image of synthesized catalysts (a, b) Ni20CGO, (c, d) Cu20CGO, (e, f) Cu40CGO, (g, h) Cu60CGO

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Fig. 3. X-ray diffraction patterns of synthesized catalysts

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Fig. 4. Comparison of methanol conversion of synthesized catalysts Ni20CGO and Cu20CGO (reaction condition:T=200-300℃, P=0-5 barg, SCR=1.5, HSV=2,000 h-1)

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Fig. 5. Catalytic performance of Ni20CGO catalyst. (a, b) yield of product gases (c, d) selectivity of product gases (reaction condition: T=200-300℃, P=0-5 barg, SCR=1.5, GHSV=2,000 h-1)

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Fig. 6. Catalytic performance of Cu20CGO catalyst. (a, b) yield of product gases (c, d) selectivity of product gases (reaction condition: T=200-300℃, P=0-5 barg, SCR=1.5, GHSV=2,000 h-1)

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Fig. 7. Comparison of Methanol conversion with Cu contents of catalysts (reaction condition : T= 200-300℃, P=0-5 barg, SCR=1.5, GHSV=2,000h-1).

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Fig. 8. Catalytic performance of Cu20CGO, Cu40CGO and Cu60CGO catalysts (a, b) 0 barg, (c, d) 2.5 barg, (e, f) 5 barg (reaction condition: T=200-300℃, SCR=1.5, GHSV=2,000 h-1)

Table 1. Summary of synthesized catalyst

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Table 2. Chemical composition of synthesized catalysts ana-lyzed by EDS

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Table 3. Characteristics of synthesized catalysts analyzed by BET, XRD

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References

  1. J. Narayana Das, "Fuel Cell Technologies for Defense Application", Energy Engineering, Springer, Singapore, 2017, pp. 9-18, doi: https://doi.org/10.1007/978-981-10-3102-1_2.
  2. A. Psoma and G. Sattler, "Fuel cell systems for submarines: from the first idea to serial production", J. Power Sources, Vol. 106, No. 1-2, 2002, pp. 381-383, doi: https://doi.org/10.1016/s0378-7753(01)01044-8.
  3. H. Ji, E. Choi, and J. Lee, "Optimal Operation Condition of Pressurized Methanol Fuel Processor for Underwater Environment", Trans. of the Korean Hydrogen and New Energy Society, Vol. 27, No. 5, 2016, pp. 485-493, doi: https://doi.org/10.7316/KHNES.2016.27.5.485.
  4. S. Krummrich and J. Llabres, "Methanol reformer - The next milestone for fuel cell powered submarines", Int. J. Hydrogen Energy, Vol. 40, No. 15, 2015, pp. 5482-5486, doi: https://doi.org/10.1016/j.ijhydene.2015.01.179.
  5. S. Sa, H. Silva, L. Brandao, J. M. Sousa, and A. Mendes, "Catalysts for methanol steam reforming-A review", Applied Catalysis B: Environmental, Vol. 99, No. 1-2, 2010, pp. 43-57, doi: https://doi.org/10.1016/j.apcatb.2010.06.015.
  6. Y. Liu, T. Hayakawa, K. Suzuki, S. Hamakawa, T. Tsunoda, T. Ishii, and M. Kumagi, "Highly active copper/ceria catalysts for steam reforming of methanol", Appl. Catal. A: General, Vol. 223, No. 1-2, 2002, pp. 137-145, doi: https://doi.org/10.1016/S0926-860X(01)00733-5.
  7. F. Tonelli, O. Gorriz, L. Arrua, and M. C. Abello, "Methanol steam reforming over Cu/$CeO_2$ catalysts. influence of zinc addition", Quim. Nova, Vol. 34, No. 8, 2011, pp. 1334-1338, doi: http://dx.doi.org/10.1590/S0100-40422011000800007.
  8. K. Ahn, Y. C. Chung, K. J. Yoon, J. W. Son, B. K. Kim, H. W. Lee, and J. H. Lee, "Lattice-strain effect of oxygen vacancy formation in gadolinium-deoped ceria", J. Electroceram., Vol. 32, No. 1, 2014, pp. 72-77, doi: https://doi.org/10.1007/s10832-013-9844-6.
  9. T. J. Huang and H. M. Chen, "Hydrogen production via steam reforming of methanol over $Cu/(Ce,Gd)O_{2-x}$ catalysts", Int. J. Hydrogen Energy, Vol. 35, 2010, pp. 6218-6226, doi: https://doi.org/10.1016/j.ijhydene.2010.03.082.
  10. S. Wongkasemjit, K. Asavaputanapun, T. Chaisuwan, and A. Luengnaruemitchai, "Steam reforming of methanol over gadolinium doped ceria (GDC) and metal loaded GDC catalysts prepared via sol-gel route", Materials Research Innovations, Vol. 16, No. 4, 2012, pp. 303-309, doi: https://doi.org/10.1179/1433075X12Y.0000000015.
  11. J. Gao, Y. Wang, Y. Ping, D. Hu, G. Xu, F. Gu, and F. Su, "A thermodynamic analysis of methanation reactions of carbon oxides for the production of synthetic natural gas", RSC Advances, Vol. 2, No. 6, 2012, pp. 2358-2368, doi: https://doi.org/10.1039/c2ra00632d.
  12. K. Stangeland, D. Kalai, H. Li, and Z. Yu, "$CO_2$ methanation: the effect of catalysts and reaction conditions", Energy Procedia, Vol. 105, 2017, pp. 2022-2027, doi: https://doi.org/10.1016/j.egypro.2017.03.577.