Cen Cente ter f r for or Dir Direc ect t Ca Cata talytic ytic Con Conver ersion sion of of Biomass Biomass to to Bi Biofu ofuels els (C3Bio) (C3Bio) C3Bio develops transformational knowledge and technologies for the direct conversion of plant lignocellulosic biomass to advanced (drop-in) biofuels and other biobased products, currently derived from oil, by the use of new chemical catalysts and thermal treatments. RESEARCH PLAN AND DIRECTIONS We will maximize the energy and carbon efficiencies of advanced biofuels production by the design of both thermal and chemical conversion processes and the biomass itself. Impacts are to more than double the carbon captured into fuel molecules and expand the product range to alkanes and other energy-rich fuels.
Ca Cata talytic ytic co conver ersion sion of of li lign gnin in Mahdi Abu-Omar and Hilkka Kenttämaa / Department of Chemistry, Purdue University Lignin is a major component of lignocellulosic O biomass. It is an aromatic rich polymer that is O O HO essential for plant’s life. Lignin poses the problem of OH OH recalcitrance as well as an opportunity for making aromatic-rich liquid fuels and valuable chemicals. A desirable catalyst is one that can depolymerize lignin, O O remove oxygens, and retain the aromaticity. Another OH OH challenge in this area is the analysis of complex 319 mixtures. We have developed a catalyst Zn/Pd/C that 100 [M-H] - cleaves aromatic ether linkages while leaving the 179 90 aromatic group unscathed. We have also implemented 80 349 mass spectrometry methods that enable the 70 quantitative analysis of lignin products. We are now 60 209 poised to apply these methods of catalysis and 50 analysis to engineered lignin biomass. 40 30 20 10 0 100 200 300 400 500 m/z
Ca Catal talyt ytic ic hy hydr drol olys ysis is of of cellulosic ma cellulosic mater terials ials & selectiv selective e oxida xidation of tion of lignin lignin mod models els C Barnes, J Abbott, D Taylor, S Chen - Univ. of Tennessee, Knoxville We are involved in the synthesis and application of organic-inorganic hybrid materials that ultimately will become single site catalysts. Using a well developed synthetic methodology, we have created high surface area catalysts functionalized with aryl sulfonic acids. These catalysts are being tested for their ability to hydrolyze cellobiose into glucose. This is a model study that has implications for the eventual conversion of cellulose from biomass into viable fuels and other high value chemicals. In a parallel line of research, we are investigating the selective oxidation of lignin models to produce quinones which may be easily transformed into value added chemicals. We are exploring a number of titanium-on-silica catalysts created through targeted synthetic methods that will allow for the determination of which active site is optimal for oxidation. Early results have been promising for conversion of the lignin models to benzoquinones in high yield and with good selectivity.
Bioc ioche hemical mical mec mecha hanism nism of of cellulose cellulose sy synth nthesis esis A Olek 1 , S Ding 2 , B Donohoe 2 , L Makowski 3 , L Paul 1 , and N Carpita 1 1 Purdue University, 2 NREL, 3 Northeastern University/ANL The 55 kDa catalytic domains of CesA spontaneously dimerize when a thiol-reducing agent is depleted from the reaction mixture. The dimerization is reversible and can be shown by high-performance size-exclusion chromatography, analytical ultracentrifugation, atomic-force microscopy, and X-ray scattering experiments. The 55 kDa monomer is predicted by WAXS to be 30.0Å, where the 110 kDa dimer is a more spherical 34.0Å. The ratio of the monomer : dimer estimates a distance between centers of mass to be 41.3Å • Synthesis of cellobiose units eliminates the steric problem of iterative synthesis of a single unit. because the O-4 would always be in the same location in the non-reducing end of the growing chain. • A channel of 8 x 2 = 16 membrane spanning domains would be equivalent to callose synthase and most sugar transport proteins. • The dimer produces two Zn-finger domains to recruit into larger complexes.
Under Underst standing anding cell w cell wall ass all assembl embly y using using Ar Arabido bidopsis psis lignin lignin mutan mutants ts J I Kim and C Chapple, Purdue University Lignin is a major component of the plant cell wall and understanding how, when and -DEX +DEX where it is deposited is critical to being C4H-deficient Control C4H-deficient able to catalyze its conversion to useful products such as biofuels. We have capitalized on our suite of lignin- deficient mutants of Arabidopsis to generate plant lines in which lignin biosynthesis, which is normally blocked in these mutants, can be turned on by application of a chemical inducer. Normally, lignin deficiency leads to dwarfing, but when lignification is induced in these lines, they again grow normally. We are now using this system to study the early stages of lignification, where lignin is first deposited and how cell wall assembly is altered when lignification is uncoupled from cell wall polysaccharide synthesis. C3 ’ H-deficient C3 ’ H-deficient Control
“Research Goes to School” An An ou outlet f tlet for or EFR EFRC C scien science ce K Clase, K Goodpaster, O Adedokun, L Kirkham, P Ertmer, G Weaver, M Abu- Omar, N Carpita, H Kenttämaa, M McCann and N Mosier, Purdue University In June 2011, 21 in-service and pre-service teachers participated in an intensive 2-week workshop From Field to Fuel - The Science of Sustainable Energy to help educators develop biofuels curricula specifically to increase the relevance of STEM subjects for rural students. “ Research Goes to School ” is an NSF Innovations through Institutional Integration grant to Purdue in collaboration with the Woodrow Wilson STEM Goes Rural Initiative, National Rural Education Association, I-STEM Resources Network, and Purdue Rural Schools Network. C3Bio investigators Abu-Omar, Carpita, Kentt ä maa, McCann and Mosier assisted Dr. Clase through presentations on their state-of-the-art research in advanced biofuels. McCann is a co-PI on the NSF grant. The teachers developed problem-based learning units for classroom curricula, mapped to educational standards using C3Bio content. The educators completed pre- and post- science teaching self-efficacy and content knowledge measures, and participated in a post-workshop focus group. Preliminary results indicate that the workshop enhanced participants ’ knowledge of biofuels concepts and their beliefs that student learning can be influenced by effective teaching. Furthermore, participants expressed that the workshop enhanced their understanding of the applications of biofuels concepts to STEM content areas and enhanced their sense of purpose for teaching.
Macr Macromolecular omolecular modeling of modeling of cellulose cellulose microf micr ofibrils fr ibrils from e om electr lectron tom on tomog ography phy P Ciesielski, J Matthews, M Crowley, M Himmel, B Donohoe (NREL) • Transmission electron tomography is used to obtain 3D data sets (tomograms) of thermochemically deconstructed plant cell walls. A single slice from a tomogram (top left) shows 2 intertwined cellulose microfibrils. • The geometry of the microfibrils is determined by fitting parametric equations to the 3D dataset (top right). • Atomistic, macromolecular models (bottom) are constructed by building the molecular structure of cellulose around the determined geometry of the microfibrils. • These structures will allow for molecular dynamics simulations that more accurately reflect the structure of biomass and are highly relevant to real processing conditions.
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