Journal
CHEMICAL ENGINEERING JOURNAL
Volume 449, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.137797
Keywords
Aryl-alcohol oxidase; Nanozyme; Hybrid catalyst; Cascade oxidation; 5-Furandicarboxylic acid
Categories
Funding
- General Programs of the National Natural Science Foundation of China [22078122]
- Major Program of National Natural Science Foundation of Jiangsu Province [19KJA150010]
- Qinglan Project of Jiangsu Province
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FDCA is a platform chemical used to produce sustainable PEF, and this study developed a catalyst that enables the efficient oxidation of HMF to FDCA. The catalyst, a hybrid of HP-7 and AAO, showed self-activation and high efficiency in the oxidation process, resulting in complete conversion of HMF with excellent selectivity.
2,5-Furandicarboxylic acid (FDCA) is a well-known biobased platform chemical to produce sustainable polyethylene furanoate (PEF) and other valuable furanic chemicals. The eco-friendly enzyme cascade reactions have been adopted to synthesize FDCA using the multistep oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) based on different oxidoreductases. However, the coordination of natural oxidoreductases in cascade reactions presents challenges because of their different adaptabilities and catalytic environments. A robust and efficient catalyst herein was developed by the hybridization of a designed hemin-peptide (HP-7) complex and natural aryl-alcohol oxidase (AAO) in iron phosphate solution to achieve the cascade oxidation of HMF to FDCA. HMF is first transformed in 5-formylfurancarboxylic acid (FFCA) based on the oxidizability of AAO toward benzylic alcohol, and then the latent activity of AAO on FFCA was activated by the catalase activity of the HP7@Fe3(PO4)2 nanozyme with the in situ consumption of H2O2 initially produced by AAO. Moreover, closer inspection demonstrated the oxidizability of the HP-7@Fe3(PO4)2 nanozyme on FFCA in both the presence and absence of H2O2 for the first time. Consequently, the hybrid catalyst AAO/HP-7@Fe3(PO4)2 enabled the selfactivated and efficient oxidation of HMF by integrating multiple reaction processes. A complete conversion of HMF with excellent selectivity (100%) toward FDCA was finally observed.
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