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Sustainable oxidative depolymerization of lignin over a ternary [VimAm]Br@POM@ACF catalyst: synergistic catalysis; solvent recyclability and life cycle assessment
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DOI：10.1039/D6NJ01320A.png)
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Abstract
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Lignin conversion into high-value aromatic monomers is severely hindered by undesired condensation; radical recombination; and poor product selectivity; restricting the sustainable substitution of fossil-derived aromatics in circular biorefineries. To overcome these challenges; a heterogeneous ternary catalyst ([VimAm] Br@POM@ACF) was fabricated by immobilizing ionic liquid-functionalized Keggin-type polyoxometalate onto KOH-treated carbon fiber cloth (ACF); integrating efficient catalytic oxidation with facile catalyst recyclability. In the oxidative depolymerization of a β-O-4 lignin model compound using H2O2 as a green oxidant; the optimized catalyst achieved 72.73% substrate conversion and 19.94% total aromatic monomer yield; with high selectivity to methyl mandelate (67.65%) and methyl benzoate (29.94%). The catalyst exhibited exceptional recyclability over five cycles; with minimal activity loss and ultra-low metal leaching. Compared with homogeneous catalysts; the ternary catalyst exhibited negligible metal leaching; and the methanol/water solvent system achieved >80% recovery after three cycles; reducing the process E-factor from 8.5 to 5.2. A cradle-to-gate life cycle assessment (LCA) identified the synthesis of POM and ionic liquid as the primary environmental hotspots; contributing significantly to global warming potential (526.87 kg CO2 eq kg−1 catalyst) and primary energy demand (6930 MJ kg−1 catalyst). To our knowledge; this is the first report of a macroscopic ACF-supported IL-POM ternary catalyst for oxidative lignin depolymerization; and the first to couple catalytic performance with solvent recyclability; E-factor analysis; and LCA for this material class. This study not only presents a highly efficient and recyclable catalyst for lignin depolymerization but also provides a quantitative environmental profile and a roadmap for green optimization; advancing the sustainable upgrading of lignin toward a circular bioeconomy.
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