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 |
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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. |
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ISSN: | 2041-1723 2041-1723 |
DOI: | 10.1038/s41467-022-30411-7 |