Dataset Information

A Convergent Approach for a Deep Converting Lignin-First Biorefinery Rendering High-Energy-Density Drop-in Fuels.

ABSTRACT: Herein, a lignin-centered convergent approach to produce either aliphatic or aromatic bio-hydrocarbons is introduced. First, poplar or spruce wood was deconstructed by a lignin-first biorefining process, a technique based on the early-stage catalytic conversion of lignin, yielding lignin oils along with cellulosic pulps. Next, the lignin oils were catalytically upgraded in the presence of a phosphidated Ni/SiO2 catalyst under H2 pressure. Notably, selectivity toward aliphatics or aromatics can simply be adjusted by changes in H2 pressure and temperature. The process renders two distinct main cuts of branched hydrocarbons (gasoline: C6-C10, and kerosene/diesel: C14-C20). As the approach is H2-intensive, we examined the utilization of pulp as an H2 source via gasification. For several biomass sources, the H2 obtainable by gasification stoichiometrically meets the H2 demand of the deep converting lignin-first biorefinery, making this concept plausible for the production of high-energy-density drop-in biofuels.

SUBMITTER: Cao Z

PROVIDER: S-EPMC6015120 | biostudies-literature | 2018 Jun

REPOSITORIES: biostudies-literature

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A Convergent Approach for a Deep Converting Lignin-First Biorefinery Rendering High-Energy-Density Drop-in Fuels.

Cao Zhengwen Z Dierks Michael M Clough Matthew Thomas MT Daltro de Castro Ilton Barros IB Rinaldi Roberto R

Joule 20180620 6

Herein, a lignin-centered convergent approach to produce either aliphatic or aromatic bio-hydrocarbons is introduced. First, poplar or spruce wood was deconstructed by a lignin-first biorefining process, a technique based on the early-stage catalytic conversion of lignin, yielding lignin oils along with cellulosic pulps. Next, the lignin oils were catalytically upgraded in the presence of a phosphidated Ni/SiO<sub>2</sub> catalyst under H<sub>2</sub> pressure. Notably, selectivity toward aliphat ...[more]

PMID: 29955733

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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.

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.

Dataset Information

A Convergent Approach for a Deep Converting Lignin-First Biorefinery Rendering High-Energy-Density Drop-in Fuels.

Publications

A Convergent Approach for a Deep Converting Lignin-First Biorefinery Rendering High-Energy-Density Drop-in Fuels.

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