Abstract
Most existing CO2 conversion processes use pure CO2 that comes from CO2 recovery, separation and subsequent purification, which are all energy- consuming steps that add up the cost and can lead to additional CO2 emission. A novel process concept, tri-reforming, is proposed for effective conversion and utilization of CO2 in the flue gases from fossil fuel-based power plants in the 21st century. The CO2, H2O, and O2 in the waste flue gas need not be pre-separated because they will be used as co-reactants for tri-reforming of natural gas. The tri-reforming is a synergetic combination of CO2 reforming, steam reforming, and partial oxidation of natural gas. The simultaneous oxy-CO2-steam reforming reactions in the tri-reforming process can produce synthesis gas (CO+H2) with H2/CO ratios (1.5–2.0) and can also eliminate carbon formation which is a serious problem in the CO2 reforming of methane. These two advantages have been demonstrated by a preliminary laboratory experimental study of tri-reforming in comparison to CO2 reforming at 850°C. A comparative analysis by calculation indicated that tri-reforming is more desired for producing syngas with H2/CO ratios of 2.0 compared to CO2 reforming and steam reforming of methane. The tri-reforming process could be applied, in principle, to the natural gas-based power plants and coal-based power plants. The syngas with desired H2/CO ratios can be used for synthesis of chemicals (alcohol, ether, olefins, etc.), ultra-clean fuels (hydrocarbon fuels and oxygenated fuels), and could also be used for generating electricity.
Access this chapter
Tax calculation will be finalised at checkout
Purchases are for personal use only
Preview
Unable to display preview. Download preview PDF.
References
Halmann, M. M.; Steinberg, M. Greenhouse Gas Carbon Dioxide Mitigation: Science and Technology. Lewis Publishers, Boca Raton, FL, 1999, 568 pp.
DOE/OS-FE. Carbon Sequestration. State of the Science. Office of Science and Office of Fossil Energy, U.S. DOE, 1999.
Weimer, T., Schaber, K., Specht, M. and Bandi, A. Comparison of CO2-Sources for Fuel Synthesis. Am. Chem. Soc. Div. Fuel Chem. Prepr., 1996, 41 (4), 1337–1340.
DOE/FE. Capturing Carbon Dioxide. Office of Fossil Energy, U.S. DOE, 1999.
EIA/IEO. International Energy Outlook (IEO), Energy Information Administration, U.S. DOE, 1999.
EIA/AER. Annual Energy Review (AER) 1998, Energy Information Administration, U.S. DOE, 1999.
Miller, B. and Pisupati, S. Personal Communication on Power Plants and Flue Gases. Pennsylvania State University, November 24, 1999.
Rostrup-Nielsen JR. Production of Synthesis Gas. Catal. Today, 1993, 18 (4), 305–324.
Armor J.N. The multiple Roles for Catalysis in the Production of H2. Appl. Catal. A: General, 1999, 176, 159–176.
Gunardson, H.H. and Abrardo, J.M. Produce CO-rich Synthesis Gas. Hydrocarbon Processing, 1999, 78 (4), 87–93.
Gunardson, H. Industrial Gases in Petrochemical Processing. Marcel Dekker, New York, 1998,283 pp.
Ashcroft A. T., Cheetham A. K., Green M. L.H., Vernon P.D.F. Partial Oxidation of Methane to Synthesis Gas Using Carbon Dioxide. Nature, 1991, 352 (6332), 225–226.
Rostrup-Nielsen JR. and Hansen J.H.B. J. CO2-Reforming of Methane over Transition Metals. Catal., 1993, 144 (1), 38–49.
Wang, S., G. Q. Lu, and G. J. Miller. Carbon Dioxide Reforming of Methane to Produce Synthesis Gas over Metal-Supported Catalysts: State of the Art. Energy & Fuels, 1996, 10,896–904.
Bradford M.C.J. and Vannice M.A. CO2 Reforming of CH4. Catal. Rev., 1999, 41 (1), 1–42
O’Connor A.M. and Ross J.R.H. The Effect of O2 Addition on the Carbon Dioxide Reforming of Methane over Pt/ZrO2 Catalysts. Catal. Today, 1998, 46 (2–3), 203–210.
Teuner S. A New Process to Make OXO-Feed. Hydrocarbon Process., 1987, 66 (7), 52–52.
Kurz G. and Teuner S. CALCOR Process for CO Production. ERDOL KOHLE ERDGAS P., 1990, 43 (5), 171 –172.
Song, C., Srinivas, S.T., Sun, L., and Armor, J.N. Comparison of High-pressure and Atmospheric-pressure Reactions for CO2 Reforming of CH4 over Ni/Na-Y and Ni/Al2O3 Catalysts. Am. Chem. Soc. Div. Petrol. Chem. Prepr., 2000, 45 (1), 143–148.
Srinivas, S. T., Song, C., Pan, W. and Sun, L. Am. Chem. Soc. Div. Petrol. Chem. Prepr., 2000, 45 (2), 348–351.
Tomishige, K., Himeno, Y., Matsuo, Y., Yoshinaga, Y0., Fujimoto, K. Catalytic Performance and Carbon Deposition Behavior of a NiO-MgO Solid Solution in Methane Reforming with Carbon Dioxide under Pressurized Conditions. Ind. Eng. Chem. Res., 2000, 39 (6), 1891–1897
Dissanayake, D., Rosynek M.P., Kharas K.C.C. and Lunsford J.H. Partial Oxidation of Methane to Carbon-Monoxide and Hydrogen over a Ni/Al2O3 Catalyst. J. Catal., 1991, 132(1), 117–127.
Hickman D.A., Haupfear E.A., and Schmidt L.D. Synthesis Gas Formation by Direct Oxidation of Methane over Rh Monoliths. Catal. Lett., 1993, 17 (3–4), 223–237.
Pena M.A., Gomez J.P., and Fierro J.L.G. New Catalytic Routes for Syngas and Hydrogen Production. Appl. Catal. A: Gen., 1996, 144 (1–2), 7–57.
Ruckenstein E. and Hu Y. H. Combination of CO2 reforming and partial oxidation of methane over NiO/MgO solid solution catalysts. Ind. Eng. Chem. Res., 1998, 37 (5), 1744–1747.
Song, C. Chemicals, Fuels and Electricity Co-generated from Coal. A Proposed Concept for Utilization of CO2 from Power Plants. Proc. 16th Annual International Pittsburgh Coal Conference, Pittsburgh, PA, October 11–15, 1999, Paper No. 16–5.
Song, C. A Proposed Concept for CO2-Based Tri-generation of Chemicals, Fuels and Electricity. Am. Chem. Soc. Div. Petrol. Chem. Prepr., 2000, 45 (1), 159–163.
DOE/FE. Project Facts-Advanced Power and Fuel Technologies. The Vision 21 EnergyPlex Concept. DOE/FE-0364, Office of Fossil Energy, U.S. DOE, 1999.
DOE/FETC. Vision 21 Program Plan-Clean Energy Plants for the 21st Century. Federal Energy Technology Center, Office of Fossil Energy, U.S. DOE, 1999c.
Pan, W., Srinivas, T.S. and Song, C. CO2 Reforming and Steam Reforming of Methane at Elevated Pressures : A Computational Thermodynamic Study. Proc. 16th Annual International Pittsburgh Coal Conference, Pittsburgh, PA, October 11–15, 1999, Paper No. 26–2.
Pan, W., and Song, C. Computational Analysis of Energy Aspects of CO2 Reforming and Oxy-CO2 Reforming of Methane at High Pressure. Am. Chem. Soc. Div. Petrol. Chem. Prepr., 2000, 45(1), 168–171.
Vernon, P.D.F., Green, M.L.H., Cheetham, A.K., Ashcroft, A.T.. Partial Oxidation of Methane to Synthesis Gas, and Carbon-Dioxide as an Oxidizing-Agent for Methane Conversion. Catal. Today,, 1992, 13 (2–3), 417–426.
Choudhary V.R., Rajput A.M., and Prabhakar B. Energy-Efficient Methane-to- Syngas Conversion with Low H2/CO Ratio by Simultaneous Catalytic Reactions of Methane with Carbon-Dioxide and Oxygen. Catal. Lett., 1995, 32 (3–4), 391–396.
Choudhary, V.R.; Mamman, A. S. Simultaneous Oxidative Conversion and CO2 or Steam Reforming of Methane to Syngas over CoO-NiO-MgO Catalyst. J. Chem. Technol. Biotechnol., 1998, 73 (4), 345–350.
Tjatjopoulos, G. J. and Vasalos, I. A. Feasibility Analysis of Ternary Feed Mixtures of Methane with Oxygen, Steam, and Carbon Dioxide for the Production of Methanol Synthesis Gas. Ind. Eng. Chem. Res., 1998,37, 1410–1421.
Inui T., Saigo K., Fujii Y., and Fujioka K. Catalytic Combustion of Natural Gas as the Role of On-site Heat Supply in Rapid Catalytic CO2-H2O Reforming of Methane. Catal. Today,, 1995, 26 (3–4), 295–302.
Choudhary V.R., Rajput A.M., and Prabhakar B. NiO/CaO-Catalyzed Formation of Syngas by Coupled Exothermic Oxidation Conversion and Endothermic CO2 and Steam Reforming of Methane, Angew. Chem. Int. Ed. Engl., 1994, 33 (20), 2104–2106.
Choudhary, V. R., and Rajput A.M. Simulataneous Carbon Dioxide and Steam Reforming of Methane to Syngas over NiO-CaO Catalyst. Ind. Eng. Chem. Res., 1996,35,3934–3939.
Choudhary, V.R.; Uphade, B.S., Mamman, A. S. Simultaneous Steam and CO2 or Reforming of Methane to Syngas over NiO/MgO/SA-5205 in Presence and Absence of Oxygen. Appl. Catal. A: Gen., 1998, 168, 33–46.
Hegarty M.E.S., O’Connor A.M. and Ross J.R.H. Syngas Production from Natural Gas using ZrO2-Supported metals. Catal. Today, 1998, 42 (3), 225–232.
Song, C., Srinivas, ST., Pan, W. and Sun, L. Technical Program, 17th North American Catalysis Society Meeting, Toronto, Canada, June 3–8, 2001.
Payner, R., Chen, S.L., Wolsky, A.M., Richter, W.F. CO2 Recovery via Coal Combustion in Mixtures of Oxygen and Recycled Flue Gas. Combust. Sci. Technol., 1989,67(1–3), 1–16.
Nakayama, S., Noguchi, Y., Kiga, T., Miyamae, S., Maeda U., Kawai M., Tanaka, T., Koyata, K., Makino, H. Pulverized Coal Combustion in O2-CO2 Mixtures on a Power Plant for CO2 Recovery. Energy Conv. Manage., 1992, 33 (5–8), 379–386.
Kiga T, Takano S, Kimura N, Omata K, Okawa M, Mori T, Kato M. Characteristics of pulverized-coal combustion in the system of oxygen recycled flue gas combustion. Energy Conv. Manage., 1997, 38, S129-S134.
Chiesa P, Lozza G . CO2 emission abatement in IGCC power plants by semiclosed cycles: Part A - With oxygen-blown combustion. J. Eng. Gas Turbines Power-Trans. ASME, 1999, 121 (4), 635–641.
Croiset, E., Thambimuthu, K., Palmer, A. Coal Combustion in O2/CO2 Mixtures Compared with Air. Can. J. Chem. Eng., 2000, 78 (2), 402–407.
Hosoda H, Hirama T, Azuma N, Kuramoto K, Hayashi J, Chiba T. NOx and N2O emission in bubbling fluidized-bed coal combustion with oxygen and recycled flue gas: Macroscopic characteristics of their formation and reduction. Energy Fuel, 1998, 12(1), 102–108.
Jager, B. Developments in Fischer-Tropsch Technology. Stud. Surf. Sci. Catal., 1998, 119,25–34.
Zhang, Y.-Q.; Davis, B. H. Indirect Coal Liquefaction - Where Do We Stand? Proceedings of 15th Ann. Internat. Pittsburgh Coal Conf., Pittsburgh, Sept 14–18, 1998, paper No. 26–6.
Senden M. M. G., Punt A. D., Hoek A. Gas-to-liquids processes: Current status & future prospects. STUD SURF SCI CATAL, 1998, 119, 961–966.
Venkataraman VK, Guthrie HD, Avellanet RA, Driscoll DJ. Overview of US DOE’s natural gas-to-liquids RD & D program and commercialization strategy. Stud. Surf Sci. Catal., 1998, 119,913–918.
Bhatt, B. L.; Heydorn, E. C.; Tijm, P. J. A.; Street, B. T.; Kornosky, R. M. Liquid Phase Methanol (LPMEOH™) Process Development. Am. Chem. Soc. Div. Petrol. Chem. Prepr., 1999, 44 (1), 25–27.
Vanliere, J., Bakker, W.T. Coal-Gasification for Electric Power Generation. Materials at High Temperatures. 1993, 11 (1–4), 4–9.
Cavallaro, S„ Freni, S. Syngas and Electricity Production by an Integrated Autothermal Reforming/Molten Carbonate Fuel Cell System. J. Power Sources, 1998,76(2), 190–196.
Vollmar, H.E., Maier, C.U., Nolscher, C., Merklein, T., Poppinger, M. Innovative Concepts for the Coproduction of Electricity and Syngas with Solid Oxide Fuel Cells. J. Power Sources, 2000, 86 (1–2), 90–97.
Author information
Authors and Affiliations
Editor information
Editors and Affiliations
Rights and permissions
Copyright information
© 2002 Springer Science+Business Media New York
About this chapter
Cite this chapter
Song, C., Pan, W., Srimat, S.T. (2002). Tri-reforming of Natural Gas Using CO2 in Flue Gas of Power Plants without CO2 Pre-separation for Production of Synthesis Gas with Desired H2/CO Ratios. In: Maroto-Valer, M.M., Song, C., Soong, Y. (eds) Environmental Challenges and Greenhouse Gas Control for Fossil Fuel Utilization in the 21st Century. Springer, Boston, MA. https://doi.org/10.1007/978-1-4615-0773-4_18
Download citation
DOI: https://doi.org/10.1007/978-1-4615-0773-4_18
Publisher Name: Springer, Boston, MA
Print ISBN: 978-1-4613-5232-7
Online ISBN: 978-1-4615-0773-4
eBook Packages: Springer Book Archive