Hierarchical Porous Metal–Organic Polyhedra for Efficient Oxidative Cleavage of β-O-4 Bonds in Lignin Model Compound
Year: 2024
Type: article
Abstract: Catalytic cleavage of β-O-4 linkages is an essential but challenging step in the depolymerization of lignin. Here, we report the templated electrosynthesis of a hydrophobic metal–organic polyhedral catalyst (Cu-MOP-e), which exhibits excellent hydrothermal stability and exceptional activity for this reaction. The oxidative cleavage of 2-phenoxyacetophenone, 1, a lignin model compound, over Cu-MOP-e at 90 °C for 1 h affords full conversion with yields of the monomer products phenol and benzoic acid of 99%. The reusability of Cu-MOP-e was confirmed by carrying out ten cycles of reaction. The mechanism of catalyst-substrate binding was investigated by high-resolution synchrotron X-ray powder diffraction, in situ X-ray absorption spectroscopy, electron paramagnetic resonance spectroscopy, and density functional theory (DFT) calculations. The combination of optimal porosity and active Cu(II) sites provides confined binding of 2-phenoxyacetophenone, thus promoting the cleavage of β-O-4 linkage under relatively mild conditions.
Source: CCS Chemistry
Institutions: Chinese Academy of Sciences, University of Manchester, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Rutherford Appleton Laboratory, Research Complex at Harwell, UK Catalysis Hub, Cardiff University, Beijing Normal University, University of Glasgow, University College London, Peking University
Language: English
Topic: Lignin and Wood Chemistry
Subfield: Biomedical Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: diamond
Awards: G1942994768, G4581035372
OpenAlex ID: W4405660498