Dihydroxyacetone valorization with high atom efficiency via controlling radical oxidation pathways over natural mineral-inspired catalyst

Jinling Wang, Xingchao Dai, Hualin Wang, Honglai Liu, Jabor Rabeah, Angelika Brückner (), Feng Shi, Ming Gong and Xuejing Yang ()
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Jinling Wang: East China University of Science and Technology (ECUST)
Xingchao Dai: Leibniz-Institut für Katalyse e.V. an der Universität Rostock (LIKAT)
Hualin Wang: East China University of Science and Technology (ECUST)
Honglai Liu: State Key Laboratory of Chemical Engineering, ECUST
Jabor Rabeah: Leibniz-Institut für Katalyse e.V. an der Universität Rostock (LIKAT)
Angelika Brückner: Leibniz-Institut für Katalyse e.V. an der Universität Rostock (LIKAT)
Feng Shi: Chinese Academy of Sciences
Ming Gong: Fudan University
Xuejing Yang: East China University of Science and Technology (ECUST)

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Diminishing fossil fuel resources and calls for sustainability are driving the urgent need for efficient valorization of renewable resources with high atom efficiency. Inspired from the natural goethite mineral with Mn paragenesis, we develop cost-effective MnO2/goethite catalysts for the efficient valorization of dihydroxyacetone, an important biomass-based platform molecule, into value-added glycolic acid and formic acid with 83.2% and 93.4% yields. The DHA substrates first undergo C−C cleavage to selectively form glycolic acid and hydroxymethyl (·CH2OH) radicals, which are further oxidized into formic acid. The kinetic and isotopic labeling experiments reveal that the catalase-like activity of MnO2 turns the oxidative radicals into oxygen, which then switches towards a hydroxymethyl peroxide (HMOO) pathway for formic acid generation and prevents formic acid over-oxidation. This nature-inspired catalyst design not only significantly improves the carbon efficiency to 86.6%, but also enhances the oxygen atom utilization efficiency from 11.2% to 46.6%, indicating a promising biomass valorization process.

Date: 2021
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DOI: 10.1038/s41467-021-27240-5

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