275288 Revealing Cellulose Pyrolysis Chemistry

Wednesday, October 31, 2012
Hall B (Convention Center )
Alex D. Paulsen, Chemical Engineering, University of Massachusetts Amherst, Amherst, MA, Matthew S. Mettler, Chemical Engineering, Univeristy of Delaware, Newark, DE, Dionisios G. Vlachos, Chemical Engineering, University of Delaware, Newark, DE and Paul J. Dauenhauer, Department of Chemical Engineering, University of Massachusetts-Amherst, Amherst, MA

Title: Revealing Cellulose Pyrolysis Chemistry

Authors: Alex D. Paulsen, Matthew S. Mettler, Dionisios G. Vlachos & Paul J. Dauenhauer

Abstract: Fast pyrolysis converts solid biomass to a liquid bio-oil which can be further upgraded to fuels or chemicals. This multi-step process consists of solid, liquid, gas and catalytic chemistries which must be studied independently in order to maximize insight. This work develops a kinetically-limited experimental technique for studying biomass pyrolysis and shows that glucose and cellodextrins do not behave similarly to cellulose while α-cyclodextrin does. The effect of temperature on cellulose pyrolysis products is also examined.

Additionally, we investigate secondary pyrolysis pathways within molten biomass using isotopically-labeled starting materials. Through the use of 13C-labeled sugars, we show that levoglucosan breaks down within the molten phase to form pyrans, light (C2-C3) oxygenates, and other anhydrosugars. The mechanisms of these reactions is unknown; however, we have shown using deuterated carbohydrates that levoglucosan decomposition products exhibit a distinct relationship between extent of elimination reactions and hydrogen exchange during reaction.  This demonstrates that hydrogen, which likely serves as a Brønsted catalyst within molten cellulose, plays a role in the decomposition of levoglucosan during cellulose pyrolysis.


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