Hybrid chemo-enzymatic heterogeneous catalyst for selective hydroxylation of biomass-derived molecules
(2023) Biomass to Biobased Chemicals and Materials Gordon Research conference — Location: Newry, Maine USA (26.May.2023)
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- Abstract
- In the field of biocatalysis, unspecific peroxygenases (UPO) are a promising class of enzymes featuring a large spectrum of substrates, high stability, and specificity for epoxidation and hydroxylation reactions. They allow for regio- and enantioselective functionalization in the presence of the tiniest concentrations of hydrogen peroxide while being cofactor independent1. However, they are highly susceptible to deactivation when the concentration of H2O2 increases. To alleviate this issue, gold-palladium catalysts have been developed that allow to chemo-catalytically produce H2O2 in situ at room temperature in water under low H2 and O2 pressure. Hutchings et al. have recently demonstrated that combining the Au-Pd catalysts and UPO enabled the one-pot one-step cascade reactions in such conditions with no interference between the inorganic and biological catalysts2. Learning from their work, and leaning on our group experience in the fabrication of hybrid chemo-enzymatic heterogeneous catalyst (HCEHC)3,4, we have successfully reproduced those Au-Pd catalysts and use them to produce the peroxide required to feed a commercial UPO. We have been able to perform with near perfect conversion and >90% selectivity the hydroxylation of propyl and ethyl benzene, two model molecules for lignin-derived substrates. We are currently expanding the scope of the process, targeting other bio-based platform molecules (terpenes, HMF5, etc.). In our ongoing work we strive to immobilize the enzyme inside a modified Au-Pd-based catalyst, to effectively create a bifunctional hybrid catalyst able to perform the same cascade reaction. We ambition to develop a catalyst that is fully recoverable and reusable, paving the way to greener oxidation processes.
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Citations
Kinnaer, M. (2023). Hybrid chemo-enzymatic heterogeneous catalyst for selective hydroxylation of biomass-derived molecules. Biomass to Biobased Chemicals and Materials Gordon Research conference, Newry, Maine USA. https://hdl.handle.net/2078.5/24114