TY - JOUR
T1 - Development of an Effective Au
T2 - Pd Bimetallic Heterogeneous Catalyst for Oxidative Lignin Depolymerization to Low Molecular Weight Aromatics
AU - Karunasinghe, Gayan
AU - Qian, Dali
AU - Meier, Mark S.
AU - Crocker, Mark
AU - Martinelli, Michela
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024/8/12
Y1 - 2024/8/12
N2 - Lignin, a phenolic-rich biomass component, holds promise for producing value-added products. However, its complex structure and recalcitrance present challenges for its effective utilization. To overcome this, a AuPd/Li−Al layered double hydroxide (LDH) catalyst was developed to facilitate lignin depolymerization. Various AuPd bimetallic nanoparticle compositions were supported on a basic Li−Al LDH support via a sol-immobilization method and characterized using N2-physisorption, X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). The catalysts were then evaluated in the oxidation of several benzylic alcohols using O2 as the oxidant, from which Au7Pd3/Li−Al LDH and Au1Pd1/Li−Al LDH were identified as possessing promising catalytic activity. Further investigations focused on the aerobic oxidation of β-O-4 linked lignin model dimers under atmospheric pressure. The tested catalysts demonstrated sequential oxidation of the model compounds, leading to cleavage of the β-O-4 linkage. Finally, the catalysts were applied to the oxidative deconstruction of γ-valerolactone (GVL) extracted maple lignin at 120 °C. Au1Pd1/Li−Al LDH emerged as the most effective catalyst, yielding a range of aromatic monomers with a total monomer yield of 27 %. These results highlight the potential of the Au1Pd1/Li−Al LDH catalyst system as an eco-friendly approach for lignin depolymerization under mild conditions.
AB - Lignin, a phenolic-rich biomass component, holds promise for producing value-added products. However, its complex structure and recalcitrance present challenges for its effective utilization. To overcome this, a AuPd/Li−Al layered double hydroxide (LDH) catalyst was developed to facilitate lignin depolymerization. Various AuPd bimetallic nanoparticle compositions were supported on a basic Li−Al LDH support via a sol-immobilization method and characterized using N2-physisorption, X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). The catalysts were then evaluated in the oxidation of several benzylic alcohols using O2 as the oxidant, from which Au7Pd3/Li−Al LDH and Au1Pd1/Li−Al LDH were identified as possessing promising catalytic activity. Further investigations focused on the aerobic oxidation of β-O-4 linked lignin model dimers under atmospheric pressure. The tested catalysts demonstrated sequential oxidation of the model compounds, leading to cleavage of the β-O-4 linkage. Finally, the catalysts were applied to the oxidative deconstruction of γ-valerolactone (GVL) extracted maple lignin at 120 °C. Au1Pd1/Li−Al LDH emerged as the most effective catalyst, yielding a range of aromatic monomers with a total monomer yield of 27 %. These results highlight the potential of the Au1Pd1/Li−Al LDH catalyst system as an eco-friendly approach for lignin depolymerization under mild conditions.
KW - Depolymerization
KW - Gold
KW - Heterogeneous catalysis
KW - Lignin
KW - Palladium
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UR - http://www.scopus.com/inward/citedby.url?scp=85200500702&partnerID=8YFLogxK
U2 - 10.1002/slct.202401532
DO - 10.1002/slct.202401532
M3 - Article
AN - SCOPUS:85200500702
VL - 9
JO - ChemistrySelect
JF - ChemistrySelect
IS - 30
M1 - e202401532
ER -