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Integrated Cascade Biorefinery Processes to Transform Woody Biomass Into Phenolic Monomers and Carbon Quantum Dots.

ABSTRACT: A novel cascade biorefinery strategy toward phenolic monomers and carbon quantum dots (CQDs) is proposed here via coupling catalytic hydrogenolysis and hydrothermal treatment. Birch wood was first treated with catalytic hydrogenolysis to afford a high yield of monomeric phenols (44.6 wt%), in which 4-propanol guaiacol (10.2 wt%) and 4-propanol syringol (29.7 wt%) were identified as the two major phenolic products with 89% selectivity. An available carbohydrate pulp retaining 82.4% cellulose and 71.6% hemicellulose was also obtained simultaneously, which was further used for the synthesis of CQDs by a one-step hydrothermal process. The as-prepared CQDs exhibited excellent selectivity and detection limits for several heavy metal cations, especially for Fe³⁺ ions in an aqueous solution. Those cost-efficient CQDs showed great potential in fluorescent sensor in situ environmental analyses. These findings provide a promising path toward developing high-performance sensors on environmental monitoring and a new route for the high value-added utilization of lignocellulosic biomass.

SUBMITTER: Chen X

PROVIDER: S-EPMC8733694 | biostudies-literature |

REPOSITORIES: biostudies-literature

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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.

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Integrated Cascade Biorefinery Processes to Transform Woody Biomass Into Phenolic Monomers and Carbon Quantum Dots.

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