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Hydrogen-enhanced catalytic hydrothermal gasification of biomass

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An Erratum to this article was published on 24 April 2017

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Abstract

The impact of hydrogen co-feeding on the catalytic hydrothermal gasification of wet biomass was explored in a continuous test rig using a feed of 10 wt% glycerol in water and a fixed bed of a carbon-supported ruthenium catalyst. The reactor was operated at a nominal temperature of 400 °C and at pressures of 26–28 MPa. Variation of the hydrogen-to-glycerol ratio as well as of the total pressure showed clearly the methanation reaction to be promoted at the expense of carbon dioxide and hydrogen formation. This is explained by a higher hydrogen surface coverage and consecutively higher rates for hydrogenation of surface-bound carbon. An increase in peak temperature of ca. 75 K occurred in the catalytic fixed-bed when co-feeding hydrogen. The measured product gas composition was close to the thermodynamic equilibrium calculated at the outlet temperature of the reactor. A maximum methane concentration of 86 vol% in the raw gas was obtained at 28 MPa with a stoichiometric addition of hydrogen. Full catalytic activity was maintained during and after the hydrogen co-feeding experiments, verified by comparing the performance of a run with a 10 wt% glycerol in water feed after co-feeding hydrogen, for which the product distribution was very close to the experiments before hydrogen co-feeding.

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  • 24 April 2017

    An erratum to this article has been published.

References

  1. Kruse A, Gawlik A (2003) Biomass conversion in water at 330−410 °C and 30−50 MPa. Identification of key compounds for indicating different chemical reaction pathways. Ind Eng Chem Res 42(2):267–279. doi:10.1021/ie0202773

    Article  Google Scholar 

  2. Schubert M, Müller JB, Vogel F (2014) Continuous hydrothermal gasification of glycerol mixtures: effect of glycerol and its degradation products on the continuous salt separation and the enhancing effect of K3PO4 on the glycerol degradation. J Supercrit Fluids 95:364–372. doi:10.1016/j.supflu.2014.09.011

    Article  Google Scholar 

  3. Elliott DC (2008) Catalytic hydrothermal gasification of biomass. Biofpr 2(3):254–265. doi:10.1002/bbb.74

    MathSciNet  Google Scholar 

  4. Elliott DC, Hart TR, Neuenschwander GG (2006) Chemical processing in high-pressure aqueous environments. 8. Improved catalysts for hydrothermal gasification. Ind Eng Chem Res 45(11):3776–3781. doi:10.1021/ie060031o

    Article  Google Scholar 

  5. Elliott DC, Sealock LJ, Baker EG (1993) Chemical processing in high-pressure aqueous environments. 2. Development of catalysts for gasification. Ind Eng Chem Res 32(8):1542–1548. doi:10.1021/ie00020a002

    Article  Google Scholar 

  6. Bagnoud-Velásquez M, Brandenberger M, Vogel F, Ludwig C (2014) Continuous catalytic hydrothermal gasification of algal biomass and case study on toxicity of aluminum as a step toward effluents recycling. Catal Today 223:35–43. doi:10.1016/j.cattod.2013.12.001

    Article  Google Scholar 

  7. Schubert M, Müller JB, Vogel F (2014) Continuous hydrothermal gasification of glycerol mixtures: autothermal operation, simultaneous salt recovery, and the effect of K3PO4 on the catalytic gasification. Ind Eng Chem Res 53(20):8404–8415. doi:10.1021/ie5005459

    Article  Google Scholar 

  8. Kruse A (2009) Hydrothermal biomass gasification. J Supercrit Fluids 47(3):391–399. doi:10.1016/j.supflu.2008.10.009

    Article  Google Scholar 

  9. Kruse A, Bernolle P, Dahmen N, Dinjus E, Maniam P (2010) Hydrothermal gasification of biomass: consecutive reactions to long-living intermediates. Energy Environ Sci 3(1):136–143. doi:10.1039/B915034J

    Article  Google Scholar 

  10. Peterson AA, Vogel F, Lachance RP, Fröling M, Antal JMJ, Tester JW (2008) Thermochemical biofuel production in hydrothermal media: a review of sub- and supercritical water technologies. Energy Environ Sci 1(1):32–65. doi:10.1039/B810100K

    Article  Google Scholar 

  11. Vogel F, Waldner MH, Rouff AA, Rabe S (2007) Synthetic natural gas from biomass by catalytic conversion in supercritical water. Green Chem 9(6):616–619. doi:10.1039/B614601E

    Article  Google Scholar 

  12. Stucki S, Vogel F, Ludwig C, Haiduc AG, Brandenberger M (2009) Catalytic gasification of algae in supercritical water for biofuel production and carbon capture. Energy Environ Sci 2(5):535–541. doi:10.1039/B819874H

    Article  Google Scholar 

  13. Kruse A, Dinjus E (2007) Hot compressed water as reaction medium and reactant: properties and synthesis reactions. J Supercrit Fluids 39(3):362–380. doi:10.1016/j.supflu.2006.03.016

    Article  Google Scholar 

  14. Brunner G (2009) Near critical and supercritical water. Part I Hydrolytic and hydrothermal processes J Supercrit Fluids 47(3):373–381. doi:10.1016/j.supflu.2008.09.002

    Article  Google Scholar 

  15. Vogel F (2010) Catalytic conversion of high-moisture biomass to synthetic natural gas in supercritical water. In: Crabtree RH (ed) Handbook of green chemistry. Handbook of green chemistry, volume 2: heterogeneous catalysis. John Wiley & Sons, Inc. doi:10.1002/9783527628698.hgc024

  16. Cortright RD, Davda RR, Dumesic JA (2002) Hydrogen from catalytic reforming of biomass-derived hydrocarbons in liquid water. Nature 418(6901):964–967. doi:10.1038/nature01009

    Article  Google Scholar 

  17. Davda RR, Shabaker JW, Huber GW, Cortright RD, Dumesic JA (2005) A review of catalytic issues and process conditions for renewable hydrogen and alkanes by aqueous-phase reforming of oxygenated hydrocarbons over supported metal catalysts. Appl Catal B-Environ 56(1–2):171–186. doi:10.1016/j.apcatb.2004.04.027

    Article  Google Scholar 

  18. Shabaker JW, Huber GW, Davda RR, Cortright RD, Dumesic JA (2003) Aqueous-phase reforming of ethylene glycol over supported platinum catalysts. Catal Lett 88(1):1–8. doi:10.1023/a:1023538917186

    Article  Google Scholar 

  19. Antal MJJ, Allen SG, Schulman D, Xu X, Divilio RJ (2000) Biomass gasification in supercritical water. Ind Eng Chem Res 39(11):4040–4053. doi:10.1021/ie0003436

    Article  Google Scholar 

  20. Vogel F (2016) Hydrothermal production of SNG from wet biomass. In: Schildhauer TJ, Biollaz SMA (eds) Synthetic natural gas from coal, dry biomass, and power-to-gas applications. John Wiley & Sons, Inc., pp 249–278. doi:10.1002/9781119191339.ch10

  21. Dreher M, Johnson B, Peterson AA, Nachtegaal M, Wambach J, Vogel F (2013) Catalysis in supercritical water: pathway of the methanation reaction and sulfur poisoning over a Ru/C catalyst during the reforming of biomolecules. J Catal 301:38–45. doi:10.1016/j.jcat.2013.01.018

    Article  Google Scholar 

  22. Peterson AA, Dreher M, Wambach J, Nachtegaal M, Dahl S, Nørskov JK, Vogel F (2012) Evidence of scrambling over ruthenium-based catalysts in supercritical-water gasification. ChemCatChem 4(8):1185–1189. doi:10.1002/cctc.201100450

    Article  Google Scholar 

  23. Peng G. (2015) Methane production from microalgae via continuous catalytic supercritical water gasification: development of catalysts and sulfur removal techniques. PhD thesis, EPFL, No. 6740

  24. Seward TM, Franck EU (1981) The system hydrogen—water up to 440°C and 2500 bar pressure. Ber Bunsenges Phys Chem 85(1):2–7. doi:10.1002/bbpc.19810850103

    Article  Google Scholar 

  25. Gassner M, Vogel F, Heyen G, Maréchal F (2011) Optimal process design for the polygeneration of SNG, power and heat by hydrothermal gasification of waste biomass: thermo-economic process modelling and integration. Energy Environ Sci 4(5):1726–1741. doi:10.1039/C0EE00629G

  26. Dreher M. (2013) Catalysis under extreme conditions: in situ studies of the reforming of organic key compounds in supercritical water. PhD thesis, ETH Zurich, No. 21531

  27. Kraft SM (2011) Modellierung und Simulation eines Festbettreaktors zur hydrothermalen Vergasung von nasser Biomasse. Master thesis, Paul Scherrer Institut/Technische Universität Wien, Vienna (Austria)

  28. Batov DV, Zaichikov AM, Slyusar VP, Korolev VP (2001) Enthalpies of mixing and state of components in aqueous-organic mixtures with nets of hydrogen bonds. Russ J Gen Chem 71(8):1208–1214. doi:10.1023/a:1013256524865

    Article  Google Scholar 

  29. Beverskog B, Puigdomenech I (1997) Revised Pourbaix diagrams for zinc at 25–300 °C. Corros Sci 39(1):107–114. doi:10.1016/S0010-938X(97)89246-3

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Acknowledgements

The authors are grateful to P. Hottinger, L. Bäni, and M. Rüttimann for technical support. Financial support in the frame of the Competence Center Energy and Mobility (CCEM project RENERG2/Future Mobility), by the Energy System Integration (ESI) Platform and the Swiss Competence Center for Energy Research (SCCER BIOSWEET), is gratefully acknowledged.

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Correspondence to S. Müller.

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The original version of this article was revised: ESM, Fig. 7, Eqs. 2, 4, and 8 have been corrected.

An erratum to this article is available at https://doi.org/10.1007/s13399-017-0260-z.

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Reimer, J., Müller, S., De Boni, E. et al. Hydrogen-enhanced catalytic hydrothermal gasification of biomass. Biomass Conv. Bioref. 7, 511–519 (2017). https://doi.org/10.1007/s13399-017-0253-y

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  • DOI: https://doi.org/10.1007/s13399-017-0253-y

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