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 () and Haotian Wang ()
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Kun Jiang: Harvard University
Seoin Back: Stanford University
Austin J. Akey: Harvard University
Chuan Xia: Harvard University
Yongfeng Hu: University of Saskatchewan
Wentao Liang: Kostas Research Institute, Northeastern University
Diane Schaak: Harvard University
Eli Stavitski: Brookhaven National Laboratory
Jens K. Nørskov: Stanford University
Samira Siahrostami: Stanford University
Haotian Wang: Harvard University

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-11992-2

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