Direct synthesis of oxalic acid via oxidative CO coupling mediated by a dinuclear hydroxycarbonylcobalt(III) complex

Yingzhuang Xu, Songyi Li and Huayi Fang ()
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Yingzhuang Xu: Tianjin Key Lab for Rare Earth Materials and Applications, Nankai University
Songyi Li: Tianjin Key Lab for Rare Earth Materials and Applications, Nankai University
Huayi Fang: Tianjin Key Lab for Rare Earth Materials and Applications, Nankai University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Oxidative coupling of CO is a straightforward and economic benign synthetic route for value-added α-diketone moiety containing C2 or higher carbon compounds in both laboratory and industry, but is still undeveloped to date. In this work, a rare coplanar dinuclear hydroxycarbonylcobalt(III) complex, bearing a Schiff-base macrocyclic equatorial ligand and a μ-κ1(O):κ1(O’)-acetate bridging axial ligand, is synthesized and characterized. The Co(III)-COOH bonds in this complex can be feasibly photocleaved, leading to the formation of oxalic acid. Moreover, the light-promoted catalytic direct production of oxalic acid from CO and H2O using O2 as the oxidant with good selectivity (> 95%) and atom economy at ambient temperature and gas pressure based on this dicobalt(III) complex have been achieved, with a turnover number of 38.5. The 13C-labelling and 18O-labelling experiments confirm that CO and H2O act as the sources of the -COOH groups in the dinuclear hydroxycarbonylcobalt(III) complex and the oxalic acid product.

Date: 2023
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DOI: 10.1038/s41467-023-38442-4

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