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Many studies of lignins in solution invoke association and aggregation phenomena to explain their solution behavior (e.g., reprecipitation onto pulp fibers, condensation, etc.). Following their colloidal (apparent) molecular weights in solution as a function of time allows us to explore observable dissociation phenomena. These measurements were carried out using multiple angle laser light scattering (MALLS) photometry in the static mode. The challenges and opportunities of measuring the specific refractive index increment (dn/dC) of lignin solutions and determining the kinetics of the dissociation process were thus investigated. Hardwood and softwood representative lignins were isolated, and method for their full dissolution in THF was further developed, which then lead to accurate dn/dC values being obtained as a function of time. When coupled to additional work using light scattering static measurements and Zimm plots for the same solutions, this effort offers insight into the aggregation and ensuing dissociative events that operate within the lignin macromolecules.

In this study, raw corn stover was subjected to dilute acid pretreatments over a range of severities under conditions similar to those identified by the National Renewable Energy Laboratory (NREL) in their techno-economic analysis of biochemical conversion of corn stover to ethanol. The pretreated corn stover then underwent enzymatic hydrolysis with yields above 70 % at moderate enzyme loading conditions. The enzyme exhausted lignin residues were characterized by ³¹P NMR spectroscopy and functional moieties quantified and correlated to enzymatic hydrolysis yields. Results from this study indicated that both xylan solubilization and lignin degradation are important for improving the enzyme accessibility and digestibility of dilute acid pretreated corn stover. At lower pretreatment temperatures, there is a good correlation between xylan solubilization and cellulose accessibility. At higher pretreatment temperatures, lignin degradation correlated better with cellulose accessibility, represented by the increase in phenolic groups. During acid pretreatment, the ratio of syringyl/guaiacyl functional groups also gradually changed from less than 1 to greater than 1 with the increase in pretreatment temperature. This implies that more syringyl units are released from lignin depolymerization of aryl ether linkages than guaiacyl units. The condensed phenolic units are also correlated with the increase in pretreatment temperature up to 180 °C, beyond which point condensation reactions may overtake the hydrolysis of aryl ether linkages as the dominant reactions of lignin, thus leading to decreased cellulose accessibility.

Approximately 89 million metric tonnes of organic chemicals and lubricants are produced annually in the United States (T.M. Carole, J. Pellegrino, and M.D. Paster. Appl. Biochem. Biotechnol. 115, 871 (2004)). The majority of these materials are fossil fuel based and may load the environment during use and at the end of their life cycle. Issues, such as disposal, pollution, and degradation, must be considered and weighed. As a result, the need to decrease pollution caused by petrochemical usage is currently impelling the development of green technologies. It is virtually inarguable that the dwindling hydrocarbon economy will eventually become unsustainable. The cost of crude oil continues to increase, while agricultural products see dramatic decreases in world market prices. These trends provide sufficient basis for renewed interest in the use of biomass as a feedstock and for the development of a carbohydrate-based economy as the logical alternative to fossil fuel resources.Résumé : Au cours d'une année, aux États-Unis d'Amérique, il se produit environ 89 millions de tonnes métriques de produits chimiques et de lubrifiants organiques. La majorité de ces produits sont obtenus à partir de combustibles fossiles et ils peuvent encrasser l'environnement durant leur cycle d'utilisation et de fin de vie. On doit donc considérer et pondérer des sujets tels que l'élimination, la pollution et la dégradation. En conséquence, la nécessité de diminuer la pollution qui est causée par l'usage des produits de l'industrie pétrochimique propulse le développement de technologies vertes. Il est pratiquement impossible de nier que l'économie basée sur les hydrocarbures ne pourra pas continuer. Le coût du brut continue d'augmenter alors que les prix des produits agricoles sur les marchés mondiaux font face à des réductions dramatiques. Ces tendances sont les bases du nouvel intérêt dans l'utilisation de la biomasse comme matière première ainsi que pour le développement d'une économie basée sur les hydrates de carbone comme alternative logique pour les ressources à base de combustibles fossiles.

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