Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination

Kun Jiang, Seoin Back, Austin J. Akey, Chuan Xia, Yongfeng Hu, Wentao Liang, Diane Schaak, Eli Stavitski, Jens K. Nørskov, Samira Siahrostami*, Haotian Wang

*Corresponding author for this work

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Abstract

Shifting electrochemical oxygen reduction towards 2e pathway to hydrogen peroxide (H2O2), instead of the traditional 4e to water, becomes increasingly important as a green method for H2O2 generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H2O2 catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm−2 H2O2 current, and a high H2O2 selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e/4e ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e, are responsible for the H2O2 pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.
Original languageEnglish
Article number3997
JournalNature Communications
Volume10
Issue number1
Number of pages11
ISSN2041-1723
DOIs
Publication statusPublished - 2019
Externally publishedYes

Cite this

Jiang, K., Back, S., Akey, A. J., Xia, C., Hu, Y., Liang, W., Schaak, D., Stavitski, E., Nørskov, J. K., Siahrostami, S., & Wang, H. (2019). Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination. Nature Communications, 10(1), [3997]. https://doi.org/10.1038/s41467-019-11992-2