期刊
NATURE COMMUNICATIONS
卷 10, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-11992-2
关键词
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资金
- Rowland Fellows Program at Rowland Institute, Harvard University
- Rice University
- National Science Foundation [ECS-0335765]
- NSERC
- National Research Council Canada
- Canadian Institutes of Health Research
- Province of Saskatchewan
- Western Economic Diversification Canada
- University of Saskatchewan
- DOE Office of Science [DE -5C0012704]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Science [DE -5C0008685]
- University of Calgary's Canada First Research Excellence Fund Program
- University of Calgary's Global Research Initiative in Sustainable Low Carbon Unconventional Resources
- Taute Lab in Rowland Institute at Harvard
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.
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