Kinetically restrained oxygen reduction to hydrogen peroxide with nearly 100% selectivity

Hydrogen peroxide has been synthesized mainly through the electrocatalytic and photocatalytic oxygen reduction reaction in recent years. Herein, we synthesize a single-atom rhodium catalyst (Rh 1 /NC) to mimic the properties of flavoenzymes for the synthesis of hydrogen peroxide under mild condition...

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Veröffentlicht in:Nature communications 2022-05, Vol.13 (1), p.2808-2808, Article 2808
Hauptverfasser: Chen, Jinxing, Ma, Qian, Zheng, Xiliang, Fang, Youxing, Wang, Jin, Dong, Shaojun
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Sprache:eng
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Zusammenfassung:Hydrogen peroxide has been synthesized mainly through the electrocatalytic and photocatalytic oxygen reduction reaction in recent years. Herein, we synthesize a single-atom rhodium catalyst (Rh 1 /NC) to mimic the properties of flavoenzymes for the synthesis of hydrogen peroxide under mild conditions. Rh 1 /NC dehydrogenates various substrates and catalyzes the reduction of oxygen to hydrogen peroxide. The maximum hydrogen peroxide production rate is 0.48 mol g catalyst −1  h −1 in the phosphorous acid aerobic oxidation reaction. We find that the selectivity of oxygen reduction to hydrogen peroxide can reach 100%. This is because a single catalytic site of Rh 1 /NC can only catalyze the removal of two electrons per substrate molecule; thus, the subsequent oxygen can only obtain two electrons to reduce to hydrogen peroxide through the typical two-electron pathway. Similarly, due to the restriction of substrate dehydrogenation, the hydrogen peroxide selectivity in commercial Pt/C-catalyzed enzymatic reactions can be found to reach 75%, which is 30 times higher than that in electrocatalytic oxygen reduction reactions. The electrocatalytic oxygen reduction reaction has been investigated in recent years for the production of H 2 O 2 from O 2 . In this article, the authors report a single-atom rhodium catalyst, based on the Flavin-dependent oxidase, for this transformation.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-022-30411-7