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      Integrating lignin depolymerization with microbial funneling processes using agronomically relevant feedstocks

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          Abstract

          This work shows the integration of reductive lignin depolymerization and microbial funneling with Novosphingobium aromaticivorans to produce 2-pyrone-4,6-dicarboxylic acid (PDC) in a lignocellulosic biorefinery.

          Abstract

          The economic feasibility of the lignocellulosic biomass refinery requires the valorization of lignin in addition to its polysaccharide fraction. One promising approach is the combination of chemical methods for lignin fractionation and depolymerization with microbial funneling of the resulting phenolic monomers into valuable chemicals. In this work, we explored the integration of γ-valerolactone (GVL) for biomass pretreatment, catalytic hydrogenolysis for lignin depolymerization, and microbial funneling to 2-pyrone-4,6-dicarboxylic acid (PDC) by the engineered bacterium Novosphingobium aromaticivorans strain PDC. We first investigated the microbial PDC production feasibility from common phenolic compounds previously identified in lignin hydrogenolysis products. Next, we studied the PDC production potential from maple, poplar, sorghum, and switchgrass using the proposed integrated pipeline and, finally, we performed a technoeconomic analysis (TEA) of the system to identify parameters that affect its economic feasibility. We found that N. aromaticivorans strain PDC is able to produce PDC from phenolic compounds with propanol, methyl, or methyl ester sidechains. Using Pd/C as a catalyst for hydrogenolysis to favor the production of these phenolics from lignin extracted with the GVL process, we obtained microbial PDC production yields of 88, 139, 103, and 79 g PDC per kg lignin from maple, poplar, sorghum, and switchgrass, respectively. Using these yields, we estimated a baseline minimum selling price of $12.10 per kg of purified PDC, and identified options to further improve the integrated pipeline.

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          Most cited references63

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          Lignin valorization: improving lignin processing in the biorefinery.

          Research and development activities directed toward commercial production of cellulosic ethanol have created the opportunity to dramatically increase the transformation of lignin to value-added products. Here, we highlight recent advances in this lignin valorization effort. Discovery of genetic variants in native populations of bioenergy crops and direct manipulation of biosynthesis pathways have produced lignin feedstocks with favorable properties for recovery and downstream conversion. Advances in analytical chemistry and computational modeling detail the structure of the modified lignin and direct bioengineering strategies for future targeted properties. Refinement of biomass pretreatment technologies has further facilitated lignin recovery, and this coupled with genetic engineering will enable new uses for this biopolymer, including low-cost carbon fibers, engineered plastics and thermoplastic elastomers, polymeric foams, fungible fuels, and commodity chemicals.
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            The catalytic valorization of lignin for the production of renewable chemicals.

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              Chemicals from lignin: an interplay of lignocellulose fractionation, depolymerisation, and upgrading.

              In pursuit of more sustainable and competitive biorefineries, the effective valorisation of lignin is key. An alluring opportunity is the exploitation of lignin as a resource for chemicals. Three technological biorefinery aspects will determine the realisation of a successful lignin-to-chemicals valorisation chain, namely (i) lignocellulose fractionation, (ii) lignin depolymerisation, and (iii) upgrading towards targeted chemicals. This review provides a summary and perspective of the extensive research that has been devoted to each of these three interconnected biorefinery aspects, ranging from industrially well-established techniques to the latest cutting edge innovations. To navigate the reader through the overwhelming collection of literature on each topic, distinct strategies/topics were delineated and summarised in comprehensive overview figures. Upon closer inspection, conceptual principles arise that rationalise the success of certain methodologies, and more importantly, can guide future research to further expand the portfolio of promising technologies. When targeting chemicals, a key objective during the fractionation and depolymerisation stage is to minimise lignin condensation (i.e. formation of resistive carbon-carbon linkages). During fractionation, this can be achieved by either (i) preserving the (native) lignin structure or (ii) by tolerating depolymerisation of the lignin polymer but preventing condensation through chemical quenching or physical removal of reactive intermediates. The latter strategy is also commonly applied in the lignin depolymerisation stage, while an alternative approach is to augment the relative rate of depolymerisation vs. condensation by enhancing the reactivity of the lignin structure towards depolymerisation. Finally, because depolymerised lignins often consist of a complex mixture of various compounds, upgrading of the raw product mixture through convergent transformations embodies a promising approach to decrease the complexity. This particular upgrading approach is termed funneling, and includes both chemocatalytic and biological strategies.
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                Journal
                GRCHFJ
                Green Chemistry
                Green Chem.
                Royal Society of Chemistry (RSC)
                1463-9262
                1463-9270
                April 04 2022
                2022
                : 24
                : 7
                : 2795-2811
                Affiliations
                [1 ]Department of Civil and Environmental Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, USA
                [2 ]Wisconsin Energy Institute, University of Wisconsin-Madison, Madison, Wisconsin 53726, USA
                [3 ]Great Lakes Bioenergy Research Center, University of Wisconsin-Madison, Madison, Wisconsin 53726, USA
                [4 ]Andlinger Center for Energy and the Environment, Princeton University, Princeton, NJ, 08544, USA
                [5 ]Department of Chemical and Biological Engineering, Princeton University, Princeton, New Jersey 08544, USA
                [6 ]Department of Biochemistry, University of Wisconsin-Madison, Madison, Wisconsin 53726, USA
                [7 ]Department of Bacteriology, University of Wisconsin-Madison, Madison, Wisconsin 53706, USA
                Article
                10.1039/D1GC03592D
                57391059-820c-4f3e-9e8c-93db9615b939
                © 2022

                http://creativecommons.org/licenses/by-nc/3.0/

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