Dataset Information

Toward a Consolidated Lignin Biorefinery: Preserving the Lignin Structure through Additive-Free Protection Strategies.

ABSTRACT: As part of the continuing efforts in lignin-first biorefinery concepts, this study concerns a consolidated green processing approach to obtain high yields of hemicelluloses and lignin with a close to native molecular structure, leaving a fiber fraction enriched in crystalline cellulose. This is done by subcritical water extraction of hemicelluloses followed by organosolv lignin extraction. This initial report focuses on a detailed characterization of the lignin component, with the aim of unravelling processing strategies for the preservation of the native linkages while still obtaining good yields and high purity. To this effect, a static cycle process is developed as a physical protection strategy for lignin, and advanced NMR analysis is applied to study structural changes in lignin. Chemical protection mechanisms in the cyclic method are also reported and contrasted with the mechanisms in a reference batch extraction process where the role of homolytic cleavage in subsequent repolymerization reactions is elucidated.

SUBMITTER: Karlsson M

PROVIDER: S-EPMC7540675 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Toward a Consolidated Lignin Biorefinery: Preserving the Lignin Structure through Additive-Free Protection Strategies.

Karlsson Maria M Giummarella Nicola N Lindén Pär A PA Lawoko Martin M

ChemSusChem 20200630 17

As part of the continuing efforts in lignin-first biorefinery concepts, this study concerns a consolidated green processing approach to obtain high yields of hemicelluloses and lignin with a close to native molecular structure, leaving a fiber fraction enriched in crystalline cellulose. This is done by subcritical water extraction of hemicelluloses followed by organosolv lignin extraction. This initial report focuses on a detailed characterization of the lignin component, with the aim of unravel ...[more]

PMID: 32530110

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Project description:BackgroundLow-temperature swelling of cotton linter cellulose and subsequent gelatinization in trifluoroacetic acid (TFA) greatly enhance rates of enzymatic digestion or maleic acid-AlCl3 catalyzed conversion to hydroxymethylfurfural (HMF) and levulinic acid (LA). However, lignin inhibits low-temperature swelling of TFA-treated intact wood particles from hybrid poplar (Populus tremula?×?P. alba) and results in greatly reduced yields of glucose or catalytic conversion compared to lignin-free cellulose. Previous studies have established that wood particles from transgenic lines of hybrid poplar with high syringyl (S) lignin content give greater glucose yields following enzymatic digestion.ResultsLow-temperature (-?20 °C) treatment of S-lignin-rich poplar wood particles in TFA slightly increased yields of glucose from enzymatic digestions and HMF and LA from maleic acid-AlCl3 catalysis. Subsequent gelatinization at 55 °C resulted in over 80% digestion of cellulose in only 3 to 6 h with high-S-lignin wood, compared to 20-60% digestion in the wild-type poplar hybrid and transgenic lines high in guaiacyl lignin or 5-hydroxy-G lignin. Disassembly of lignin in woody particles by Ni/C catalytic systems improved yields of glucose by enzymatic digestion or catalytic conversion to HMF and LA. Although lignin was completely removed by Ni/C-catalyzed delignification (CDL) treatment, recalcitrance to enzymatic digestion of cellulose from the high-S lines was reduced compared to other lignin variants. However, cellulose still exhibited considerable recalcitrance to complete enzymatic digestion or catalytic conversion after complete delignification. Low-temperature swelling of the CDL-treated wood particles in TFA resulted in nearly complete enzymatic hydrolysis, regardless of original lignin composition.ConclusionsGenetic modification of lignin composition can enhance the portfolio of aromatic products obtained from lignocellulosic biomass while promoting disassembly into biofuel and bioproduct substrates. CDL enhances rates of enzymatic digestion and chemical conversion, but cellulose remains intrinsically recalcitrant. Cold TFA is sufficient to overcome this recalcitrance after CDL treatment. Our results inform a 'no carbon left behind' strategy to convert total woody biomass into lignin, cellulose, and hemicellulose value streams for the future biorefinery.

Project description:Background:Lignocellulosic biomass has long been recognized as a potential sustainable source for industrial applications. The costs associated with conversion of plant biomass to fermentable sugar represent a significant barrier to the production of cost-competitive biochemicals. Consolidated bioprocessing (CBP) is considered a potential breakthrough for achieving cost-efficient production of biomass-based fuels and commodity chemicals. During the degradation of cellulose, cellobiose (major end-product of cellulase activity) is catabolized by hydrolytic and phosphorolytic pathways in cellulolytic organisms. However, the details of the two intracellular cellobiose metabolism pathways in cellulolytic fungi remain to be uncovered. Results:Using the engineered malic acid production fungal strain JG207, we demonstrated that the hydrolytic pathway by ?-glucosidase and the phosphorolytic pathway by phosphorylase are both used for intracellular cellobiose metabolism in Myceliophthora thermophila, and the yield of malic acid can benefit from the energy advantages of phosphorolytic cleavage. There were obvious differences in regulation of the two cellobiose catabolic pathways depending on whether M. thermophila JG207 was grown on cellobiose or Avicel. Disruption of Mtcpp in strain JG207 led to decreased production of malic acid under cellobiose conditions, while expression levels of all three intracellular ?-glucosidase genes were significantly up-regulated to rescue the impairment of the phosphorolytic pathway under Avicel conditions. When the flux of the hydrolytic pathway was reduced, we found that ?-glucosidase encoded by bgl1 was the dominant enzyme in the hydrolytic pathway and deletion of bgl1 resulted in significant enhancement of protein secretion but reduction of malate production. Combining comprehensive manipulation of both cellobiose utilization pathways and enhancement of cellobiose uptake by overexpression of a cellobiose transporter, the final strain JG412?bgl2?bgl3 produced up to 101.2 g/L and 77.4 g/L malic acid from cellobiose and Avicel, respectively, which corresponded to respective yields of 1.35 g/g and 1.03 g/g, representing significant improvement over the starting strain JG207. Conclusions:This is the first report of detailed investigation of intracellular cellobiose catabolism in cellulolytic fungus M. thermophila. These results provide insights that can be applied to industrial fungi for production of biofuels and biochemicals from cellobiose and cellulose.

Project description:Cell growth and polyhydroxyalkanoate (PHA) biosynthesis are two key traits in PHA production from lignin or its derivatives. However, the links between them remain poorly understood. Here, the transcription levels of key genes involved in PHA biosynthesis were tracked in Pseudomonas putida strain A514 grown on vanillic acid as the sole carbon source under different levels of nutrient availability. First, enoyl-coenzyme A (CoA) hydratase (encoded by phaJ4) is stress induced and likely to contribute to PHA synthesis under nitrogen starvation conditions. Second, much higher expression levels of 3-hydroxyacyl-acyl carrier protein (ACP) thioesterase (encoded by phaG) and long-chain fatty acid-CoA ligase (encoded by alkK) under both high and low nitrogen (N) led to the hypothesis that they likely not only have a role in PHA biosynthesis but are also essential to cell growth. Third, 40 mg/liter PHA was synthesized by strain AphaJ4C1 (overexpression of phaJ4 and phaC1 in strain A514) under low-N conditions, in contrast to 23 mg/liter PHA synthesized under high-N conditions. Under high-N conditions, strain AalkKphaGC1 (overexpression of phaG, alkK, and phaC1 in A514) produced 90 mg/liter PHA with a cell dry weight of 667 mg/liter, experimentally validating our hypothesis. Finally, further enhancement in cell growth (714 mg/liter) and PHA titer (246 mg/liter) was achieved in strain Axyl_alkKphaGC1 via transcription level optimization, which was regulated by an inducible strong promoter with its regulator, XylR-PxylA, from the xylose catabolic gene cluster of the A514 genome. This study reveals genetic features of genes involved in PHA synthesis from a lignin derivative and provides a novel strategy for rational engineering of these two traits, laying the foundation for lignin-consolidated bioprocessing.IMPORTANCE With the recent advances in processing carbohydrates in lignocellulosics for bioproducts, almost all biological conversion platforms result in the formation of a significant amount of lignin by-products, representing the second most abundant feedstock on earth. However, this resource is greatly underutilized due to its heterogeneity and recalcitrant chemical structure. Thus, exploiting lignin valorization routes would achieve the complete utilization of lignocellulosic biomass and improve cost-effectiveness. The culture conditions that encourage cell growth and polyhydroxyalkanoate (PHA) accumulation are different. Such an inconsistency represents a major hurdle in lignin-to-PHA bioconversion. In this study, we traced and compared transcription levels of key genes involved in PHA biosynthesis pathways in Pseudomonas putida A514 under different nitrogen concentrations to unveil the unusual features of PHA synthesis. Furthermore, an inducible strong promoter was identified. Thus, the molecular features and new genetic tools reveal a strategy to coenhance PHA production and cell growth from a lignin derivative.

Project description:BackgroundThe production of microalgal biofuels, despite their sustainable and renowned potential, is not yet cost-effective compared to current conventional fuel technologies. However, the biorefinery concept increases the prospects of microalgal biomass as an economically viable feedstock suitable for the co-production of multiple biofuels along with value-added chemicals. To integrate biofuels production within the framework of a microalgae biorefinery, it is not only necessary to exploit multi-product platforms, but also to identify optimal microalgal cultivation strategies maximising the microalgal metabolites from which biofuels are obtained: starch and lipids. Whilst nutrient limitation is widely known for increasing starch and lipid formation, this cultivation strategy can greatly reduce microalgal growth. This work presents an optimisation framework combining predictive modelling and experimental methodologies to effectively simulate and predict microalgal growth dynamics and identify optimal cultivation strategies.ResultsMicroalgal cultivation strategies for maximised starch and lipid formation were successfully established by developing a multi-parametric kinetic model suitable for the prediction of mixotrophic microalgal growth dynamics co-limited by nitrogen and phosphorus. The model's high predictive capacity was experimentally validated against various datasets obtained from laboratory-scale cultures of Chlamydomonas reinhardtii CCAP 11/32C subject to different initial nutrient regimes. The identified model-based optimal cultivation strategies were further validated experimentally and yielded significant increases in starch (+ 270%) and lipid (+ 74%) production against a non-optimised strategy.ConclusionsThe optimised microalgal cultivation scenarios for maximised starch and lipids, as identified by the kinetic model presented here, highlight the benefits of exploiting modelling frameworks as optimisation tools that facilitate the development and commercialisation of microalgae-to-fuel technologies.

Dataset Information

Toward a Consolidated Lignin Biorefinery: Preserving the Lignin Structure through Additive-Free Protection Strategies.

Publications

Toward a Consolidated Lignin Biorefinery: Preserving the Lignin Structure through Additive-Free Protection Strategies.

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