Novel and Integrated Process for the Valorization of Kraft Lignin to Produce Lignin-Containing Vitrimers
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SUBMITTER: More A
PROVIDER: S-EPMC9835646 | biostudies-literature | 2022 Dec
REPOSITORIES: biostudies-literature
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Project description:Recent studies have found that green hydrogen production and biomass utilization technologies can be combined to efficiently produce both hydrogen and value-added chemicals using biomass as an electron and proton source. However, the majority of them have been limited to proof-of-concept demonstrations based on batch systems. Here the authors report the design of modular flow systems for the continuous depolymerization and valorization of lignin and low-voltage hydrogen production. A redox-active phosphomolybdic acid is used as a catalyst to depolymerize lignin with the production of aromatic compounds and extraction of electrons for hydrogen production. Individual processes for lignin depolymerization, byproduct separation, and hydrogen production with catalyst reactivation are modularized and integrated to perform the entire process in the serial flow. Consequently, this work enabled a one-flow process from biomass conversion to hydrogen gas generation under a cyclic loop. In addition, the unique advantages of the fluidic system (i.e., effective mass and heat transfer) substantially improved the yield and efficiency, leading to hydrogen production at a higher current density (20.5 mA cm-2 ) at a lower voltage (1.5 V) without oxygen evolution. This sustainable eco-chemical platform envisages scalable co-production of valuable chemicals and green hydrogen for industrial purposes in an energy-saving and safe manner.
| S-EPMC9762309 | biostudies-literature
Project description:Kraft lignin (KL) produced in kraft pulping process has a low molecular weight and solubility, which limits its application in industry. For the first time, KL was polymerized with acrylic acid (AA) in an acidic aqueous suspension system to produce a water soluble lignin-AA polymer with a high molecular weight in this work. The polymerization reaction was carried out using K2S2O8 as an initiator, and the influence of reaction conditions on the carboxylate group content and molecular weight of resultant lignin polymers was systematically investigated. The mechanism of polymerization of KL and AA was discussed fundamentally. The resulting lignin-AA polymer was characterized by Fourier Transform Infrared spectrophotometry (FTIR), proton nuclear magnetic resonance (1H-NMR) and elemental analyses. The results showed that the phenolic hydroxyl group (Ph-OH) content of KL promoted the polymerization under an acidic environment. Under the conditions of 1.5 wt% of initiator, 3.5 of pH, 10.0 of AA/lignin molar ratio, 0.15 mol L-1 of lignin concentration, 3 h and 80 °C, the carboxylate group content and the molecular weight of the polymer were 7.37 mmol g-1 and 7.4 × 105 g mol-1, respectively. The lignin-AA polymer was water soluble at a 10 g L-1 concentration and a pH higher than 4.5. Furthermore, the flocculation performance of lignin-AA polymer in an aluminium oxide suspension was evaluated. Compared with polyAA, the lignin-AA polymer was a more efficient flocculant for aluminium oxide suspension, which shows its potential to be used as a green flocculant in industry.
| S-EPMC9079287 | biostudies-literature
Project description:The complex chemical structure and the fact that many areas in pulping and lignin chemistry still remain unresolved are challenges associated with exploiting lignin. In this study, we address questions regarding the formation and chemical nature of the insoluble residual lignin, the presence of fatty acids in kraft lignin, and the origin of secoisolariciresinol structures. A mild thermal treatment of lignin at maximum kraft-cooking temperatures (∼170 °C) with tall oil fatty acids (TOFA) or in an inert solvent (decane) produced highly insoluble products. However, acetylation of these samples enabled detailed chemical characterization by nuclear magnetic resonance (NMR) spectroscopy. The results show that the secoisolariciresinol (β-β) structure in kraft lignin is formed by rearrangement of the β-aryl ether structure. Furthermore, fatty acids bind covalently to kraft lignin by reacting with the stilbene structures present. It is highly probable that these reactions also occur during kraft pulping, and this phenomenon has an impact on controlling the present kraft pulping process along with the development of new products from kraft lignin.
| S-EPMC8278485 | biostudies-literature
Project description:Lignin is an energy-dense, heterogeneous polymer comprised of phenylpropanoid monomers used by plants for structure, water transport, and defense, and it is the second most abundant biopolymer on Earth after cellulose. In production of fuels and chemicals from biomass, lignin is typically underused as a feedstock and burned for process heat because its inherent heterogeneity and recalcitrance make it difficult to selectively valorize. In nature, however, some organisms have evolved metabolic pathways that enable the utilization of lignin-derived aromatic molecules as carbon sources. Aromatic catabolism typically occurs via upper pathways that act as a "biological funnel" to convert heterogeneous substrates to central intermediates, such as protocatechuate or catechol. These intermediates undergo ring cleavage and are further converted via the β-ketoadipate pathway to central carbon metabolism. Here, we use a natural aromatic-catabolizing organism, Pseudomonas putida KT2440, to demonstrate that these aromatic metabolic pathways can be used to convert both aromatic model compounds and heterogeneous, lignin-enriched streams derived from pilot-scale biomass pretreatment into medium chain-length polyhydroxyalkanoates (mcl-PHAs). mcl-PHAs were then isolated from the cells and demonstrated to be similar in physicochemical properties to conventional carbohydrate-derived mcl-PHAs, which have applications as bioplastics. In a further demonstration of their utility, mcl-PHAs were catalytically converted to both chemical precursors and fuel-range hydrocarbons. Overall, this work demonstrates that the use of aromatic catabolic pathways enables an approach to valorize lignin by overcoming its inherent heterogeneity to produce fuels, chemicals, and materials.
| S-EPMC4143016 | biostudies-literature
Project description:BackgroundThe effective valorization of lignin and carbohydrates in lignocellulose matrix under the concept of biorefinery is a primary strategy to produce sustainable chemicals and fuels. Based on the reductive catalytic fractionation (RCF), lignin in lignocelluloses can be depolymerized into viscous oils, while the highly delignified pulps with high polysaccharides retention can be transformed into various chemicals.ResultsA biorefinery paradigm for sequentially valorization of the main components in poplar sawdust was constructed. In this process, the well-defined low-molecular-weight phenols and bioethanol were co-generated by tandem chemo-catalysis in the RCF stage and bio-catalysis in fermentation stage. In the RCF stage, hydrogen transfer reactions were conducted in one-pot process using Raney Ni as catalyst, while the isopropanol (2-PrOH) in the initial liquor was served as a hydrogen donor and the solvent for lignin dissolution. Results indicated the proportion of the 2-PrOH in the initial liquor of RCF influenced the chemical constitution and yield of the lignin oil, which also affected the characteristics of the pulps and the following bioethanol production. A 67.48 ± 0.44% delignification with 20.65 ± 0.31% of monolignols yield were realized when the 2-PrOH:H2O ratio in initial liquor was 7:3 (6.67 wt% of the catalyst loading, 200 °C for 3 h). The RCF pulp had higher carbohydrates retention (57.96 ± 2.78 wt%), which was converted to 21.61 ± 0.62 g/L of bioethanol with a yield of 0.429 ± 0.010 g/g in fermentation using an engineered S. cerevisiae strain. Based on the mass balance analysis, 104.4 g of ethanol and 206.5 g of lignin oil can be produced from 1000 g of the raw poplar sawdust.ConclusionsThe main chemical components in poplar sawdust can be effectively transformed into lignin oil and bioethanol. The attractive results from the biorefinery process exhibit great promise for the production of valuable biofuels and chemicals from abundant lignocellulosic materials.
| S-EPMC10800047 | biostudies-literature
Project description:BackgroundLignin is a potential feedstock for microbial conversion into various chemicals. However, the microbial degradation rate of native or technical lignin is low, and chemical depolymerization is needed to obtain reasonable conversion rates. In the current study, nine bacterial strains belonging to the Pseudomonas and Rhodococcus genera were evaluated for their ability to grow on alkaline-treated softwood lignin as a sole carbon source.ResultsPseudomonas fluorescens DSM 50090 and Rhodococcus opacus DSM1069 showed the best growth of the tested species on plates with lignin. Further evaluation of P. fluorescens and R. opacus was made in liquid cultivations with depolymerized softwood Kraft lignin (DL) at a concentration of 1 g/L. Size-exclusion chromatography (SEC) showed that R. opacus consumed most of the available lower-molecular weight compounds (approximately 0.1-0.4 kDa) in the DL, but the weight distribution of larger fractions was almost unaffected. Importantly, the consumed compounds included guaiacol-one of the main monomers in the DL. SEC analysis of P. fluorescens culture broth, in contrast, did not show a large conversion of low-molecular weight compounds, and guaiacol remained unconsumed. However, a significant shift in molecular weight distribution towards lower average weights was seen after cultivation with P. fluorescens.ConclusionsRhodococcus opacus and P. fluorescens were identified as two potential microbial candidates for the conversion/consumption of base-catalyzed depolymerized lignin, acting on low- and high-molecular weight lignin fragments, respectively. These findings will be of relevance for designing bioconversion of softwood Kraft lignin.
| S-EPMC6420747 | biostudies-literature
Project description:BackgroundLignin is a potential feedstock for microbial conversion into various chemicals. However, the degradation rate of native or technical lignin is low, and depolymerization is needed to obtain reasonable conversion rates. In the current study, base-catalyzed depolymerization-using NaOH (5 wt%)-of softwood Kraft lignin was conducted in a continuous-flow reactor system at temperatures in the range 190-240 °C and residence times of 1 or 2 min. The ability of growth of nine bacterial strains belonging to the genera Pseudomonas and Rhodococcus was tested using the alkaline-treated lignin as a sole carbon source.ResultsPseudomonas fluorescens and Rhodococcus opacus showed the best growth of the tested species on plates with lignin. Further evaluation of P. fluorescens and R. opacus was made in liquid cultivations with depolymerized lignin (DL) at a concentration of 1 g/L. Size exclusion chromatography (SEC) showed that R. opacus consumed most of the available lower molecular weight compounds (approximately 0.1-0.4 kDa) in the DL, but the weight distribution of larger fractions was almost unaffected. Importantly, the consumed compounds included guaiacol-one of the main monomers in the DL. SEC analysis of P. fluorescens culture broth, in contrast, did not show a large conversion of low molecular weight compounds, and guaiacol remained unconsumed. However, a significant shift in molecular weight distribution towards lower average weights was seen.ConclusionsRhodococcus opacus and P. fluorescens were identified as two potential microbial candidates for the conversion/consumption of base-catalyzed depolymerized lignin, acting on low and high molecular weight lignin fragments, respectively. These findings will be of relevance for designing bioconversion of softwood Kraft lignin.
| S-EPMC6123935 | biostudies-literature
Project description:Lignin, an abundant renewable resource in nature, is a highly heterogeneous biopolymer consisting of phenylpropanoid units. It is essential for sustainable utilization of biomass to convert lignin to value-added products. However, there are technical obstacles for lignin valorization due to intrinsic heterogeneity. The emerging of synthetic biology technologies brings new opportunities for lignin breakdown and utilization. In this review, we discussed the applications of synthetic biology on lignin conversion, especially the production of value-added products, such as aromatic chemicals, ring-cleaved chemicals from lignin-derived aromatics and bio-active substances. Synthetic biology will offer new potential strategies for lignin valorization by optimizing lignin degradation enzymes, building novel artificial converting pathways, and improving the chassis of model microorganisms.
| S-EPMC6999416 | biostudies-literature
Project description:The synthesis and characterisation of a lignin-based elastomer system using lignin-epoxy-resins is presented. Untreated kraft black liquor was used to synthesise glycidyl lignin or black liquor-based epoxy resin (BLER), following a published procedure. A flexible, elastomeric thermoset was produced by cross-linking BLER with succinic anhydride (SA). The produced material was characterised in respect to its chemical, thermal, mechanical and swelling characteristics. In addition, vertical burning tests were performed. The obtained lignin-based elastomeric thermoset had a tensile strength of 1.0 ± 0.20 MPa and elastic moduli of 1.6 ± 1.4 and 0.44 ± 0.35 MPa at 5% and 50% elongation, respectively. A maximum elongation of 151 ± 49% was found.
| S-EPMC11217878 | biostudies-literature
Project description:Lignin from different biomasses possess biological antioxidation and antimicrobial activities, which depend on the number of functional groups and the molecular weight of lignin. In this work, organosolv fractionation was carried out to prepare the lignin fraction with a suitable structure to tailor excellent biological activities. Gel permeation chromatography (GPC) analysis showed that decreased molecular weight lignin fractions were obtained by sequentially organosolv fractionation with anhydrous acetone, 50% acetone and 37.5% hexanes. Nuclear magnetic resonance (NMR) results indicated that the lignin fractions with lower molecular weight had fewer substructures and a higher phenolic hydroxyl content, which was positively correlated with their antioxidation ability. Both of the original lignin and fractionated lignins possessed the ability to inhibit the growth of Gram-negative bacteria (Escherichia coli and Salmonella) and Gram-positive bacteria (Streptococcus and Staphylococcus aureus) by destroying the cell wall of bacteria in vitro, in which the lignin fraction with the lowest molecular weight and highest phenolic hydroxyl content (L3) showed the best performance. Besides, the L3 lignin showed the ability to ameliorate Escherichia coli-induced diarrhea damages of mice to improve the formation of intestinal contents in vivo. These results imply that a lignin fraction with a tailored structure from bamboo lignin can be used as a novel antimicrobial agent in the biomedical field.
| S-EPMC8188334 | biostudies-literature