Utilization of renewable feedstocks is a research field of rapidly growing interest. Although a few industrial processes (e.g. ethanol from corn) have been implemented, it is clear that the long term economic viability and sustainability of these technologies require further research. Several innovative concepts have been demonstrated in the last years but many catalytic studies have only been performed with model compounds.
Our research is focused on the development of an integrated route to fuels and hydrogen from woody biomass. The first step in the chemical processing of this biomass feedstocks is depolymerization of the lignin and carbohydrate (holocellulose) fractions by aqueous phase hydrolysis. The dissolved fractions are analyzed by HPLC allowing the quantification of primary hydrolysis and degradation products. Analysis of the residues by 13 C CP MAS NMR provides information on the concentrations of lignin and carbohydrates as well as on chemical modifications that occur during the depolymerization process. This information will be important to approach the goal of complete utilization of the biomass feedstock. These initial studies will allow us to optimize the yield and selectivity to monosaccharides or other intermediates that will be used for further processing. The second part of the project will consist of the development of catalytic routes for converting depolymerized biomass into fuels. In addition to depolymerization in aqueous phase, novel reaction media are investigated for hydrolysis and reforming of biomass and model compounds. It was found that both reactions readily occur under surprisingly mild conditions.
In a second project, we investigate hydrotreating of pyrolysis oil over zeolite catalysts. We are currently building a reaction apparatus that will allow for automated sampling and temperature control.
Publications
Sievers, C., Marzialetti, T., Hoskins, T., Valenzuela, M.B., Agrawal, P.K., Jones, C.W.; “Quantitative characterization of residues from aqueous phase acid hydrolysis by solid state NMR spectroscopy” in preparation.
Sievers, C., Valenzuela, M.B., Marzialetti, T., Musin, I., Agrawal, P.K., Jones, C.W. “Ionic liquid phase hydrolysis of cellulose and pine wood” in preparation.
Sievers, C., Liebert, J.S., Stratmann M.M., Lin, X., Olindo, R., Lercher, J.A.; “Comparison of zeolites LaX and LaY as catalysts for isobutane/2-butene alkylation” Appl. Catal. A-Gen. , accepted for publication.
Sievers, C., Jiménez, O., Knapp, R., Lin, X., Müller, T.E., Türler, A., Wierczinski, B., Lercher, J.A.; “Palladium catalysts immobilized in thin films of ionic liquid for the direct addition of aniline to styrene” J. Mol. Catal. A-Chem ., available online, DOI:10.1016/j.molcata. 2007.06.016.
Fow, K.L., Jaenicke, S., Müller, T.E., Sievers, C. “ Enhanced Enantioselectivity of Chiral Hydrogenation Catalysts after Immobilisation in Thin Films of Ionic Liquid ” J. Mol. Catal. A-Chem. , available online, DOI:10.1016/j.molcata.2006.11.050.
Sievers, C., Onda, A., Guzman, A., Olindo, R., and Lercher, J.A.; “Surface chemistry of branched alkanes on lanthanum exchange zeolite X” Stud. Surf. Sci. Catal. 170 (2007) 1153.
Williams, M.F., Fonfé, B., Sievers, C., Abraham, A., van Bokhoven, J.A., Jentys, A., van Veen, J.A.R., Lercher, J.A.; “Hydrogenation of tetralin on silica-alumina supported Pt catalysts I-Physicochemical characterization of the catalytic materials” J. Catal. 251 (2007) 485.
Xu, B., Sievers, C., Lercher, J.A., van Veen, J.A.R., Giltay, P., Prins, R., van Bokhoven, J.A.; “Strong Brønsted Acidity in Amorphous Silica-Aluminas” J. Phys. Chem. C 111 (2007) 12075.
Sievers, C., Onda, A., Olindo, R., Lercher, J.A.; “ Adsorption and polarization of branched alkanes on H-LaX” J. Phys. Chem. C 111 (2007) 5454.
Sievers, C., Zuazo, I., Guzman, A., Olindo, R., Syska, H., Lercher, J.A.; “Stages of aging and deactivation of zeolite LaX in isobutane/2-butene alkylation” J. Catal. 246 (2007) 315.
Sievers, C., Onda, A., Guzman, A., Otillinger, K.S., Olindo, R., and Lercher, J.A. “Low-Temperature Activation of Branched Octane Isomers over Lanthanum Exchanged Zeolite X Catalysts” J. Phys. Chem. C 111 (2007) 210.
Guzman, A.; Zuazo, I.; Feller, A.; Olindo, R.; Sievers, C.; Lercher, J. A.; “Influence of the Activation Temperature on the Physicochemical Properties and Catalytic Activity of La-X Zeolites for Iisobutane/cis-2-Butene Alkylation” Micropor. Mesopor. Mater. 97 (2006) 49.
Xu, B., Sievers, C., Hong, S. B., Prins, R., van Bokhoven, J.A.; “ Catalytic Activity of Brønsted Acid Sites in Zeolites: Intrinsic Activity, Rate-Limiting Step, and Influence of the Local Structure of the Acid Sites” J. Catal. 244 (2006) 163.
Sievers, C., Jimenez, O., Müller, T.E., Steuernagel, S., Lercher J.A.; “ Formation of solvent cages around organometallic complexes in thin films of supported ionic liquid ” J. Am. Chem. Soc. 128 (2006) 13990.
Jimenez, O., Müller, T.E., Sievers, C., Spirkl, A., Lercher J.A.; “Markownikoff and Anti-Markownikoff Hydroamination with Palladium Catalysts Immobilized in Thin Films of Silica Supported Ionic Liquids” Chem. Comm. ( 2006) 2974 .
Guzman, A.; Zuazo, I.; Feller, A.; Olindo, R.; Sievers, C.; Lercher, J.A. “On the formation of the acid sites in lanthanum exchanged X zeolites used for isobutane/cis-2-butene alkylation” Micropor. Mesopor. Mater. 83 (2005) 309-318.
Halbach, T.S.; Mix, S.; Fischer, D.; Maechling, S.; Krause, J.O.; Sievers, C.; Blechert, S.; Nuyken, O.; Buchmeiser, M.R.J. “Novel Supported and Unsupported Ru-Based Metathesis Catalysts: Synthesis and Reactivity” J. Org. Chem. 70 (2005) 4687-4694.
Cerqueira, H.S.; Sievers, C.; Joly, G.; Magnoux, P.; Lercher, J.A. “Multitechnique Characterization of Coke Produced during Commercial Resid FCC Operation” Ind. Eng. Chem. Res. 44 (2005) 2069-2077.
Penzien, J.; Abraham, A.; van Bokhoven, J.A.; Jentys, A.; Müller, T.E.; Sievers, C.; Lercher, J.A. ”Generation and Characterization of Well-Defined Zn 2+ Lewis Acid Sites in Ion Exchanged Zeolite BEA” J. Phys. Chem. B 108 (2004) 4116-4126.
Oral Presentations
Sievers, C., Zuazo, I., Guzman, A., Olindo, R., Lercher, J.A. “Deactivation Of La-X Zeolites In isobutane/2-Butene Alkylation” Accepted for presentation at the AIChE Annual Meeting (2007). Salt Lake City, UT, USA.
Sievers, C., Marzialetti, T., Hoskins, T., Valenzuela, M.B., Agrawal, P.K., Jones, C.W. “Quantitative Solid-State NMR Characterization of Solid Residues Produced Using Different Acids in the Hydrolysis of Loblolly Pine” Accepted for presentation at the AIChE Annual Meeting (2007). Salt Lake City, UT, USA.
Sievers, C., Müller, T.E., Lercher J.A. “Novel catalytic pathways in supported ionic liquids” Accepted for presentation at the AIChE Annual Meeting (2007). Salt Lake City, UT, USA.
Sievers, C., Onda, A., Guzman, A., Olindo, R., Lercher, J.A. “Adsorption and Activation of Branched Alkanes on Zeolite LaX” Presented at the Southeastern Catalysis Society Fall Symposium (2007). Asheville, NC, USA.
Sievers, C., Liebert, J.S., Olindo, R., Lercher, J.A. “Isobutane/2-butene alkylation over lanthanum exchanged faujasite type zeolites” Presented at the 20 th North American Meeting of the North American Catalysis Society (2007). Houston, TX, USA
Sievers, C., Onda, A., Guzman, A., Olindo, R., Lercher, J.A. “Alkane activation over lanthanum exchanged zeolite X” Presented at the 20 th North American Meeting of the North American Catalysis Society (2007). Houston, TX, USA
Sievers, C., Zuazo, I., Guzman, A., Liebert, J.S., Olindo, R., Lercher, J.A. “ Isobutane/2-butene alkylation over La 3+ exchanged faujasites ” Presented at the 19. Deutsche Zeolith Tagung (2007) . Leipzig, Germany.
Sievers, C., Zuazo, I., Guzman, A., Olindo, R., Lercher, J.A. “Deposit formation and deactivation of zeolite La-X in isobutane/2-butene alkylation”. Presented at the ACS Spring Meeting (2006) . Atlanta, GA, USA.
Sievers, C., Onda, A., Guzman, A., Olindo, R., Lercher, J.A. ” In-situ study on the low temperature activation of octane isomers on H-LaX zeolites”. Presented at the 37. Jahrestreffen Deutscher Katalytiker (2005) . Weimar, Germany.
Sievers, C., Onda, A., Guzman, A., Olindo, R., Lercher, J.A. “Low Temperature Activation of Alkanes”. Presented at the 17. Deutsche Zeolith Tagung (2005) . Gießen, Germany.