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

doi:10.1038/s41467-019-11992-2

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

Nat Commun. 2019 Sep 5;10(1):3997. doi: 10.1038/s41467-019-11992-2.

Authors

Kun Jiang¹, Seoin Back², Austin J Akey³, Chuan Xia¹, Yongfeng Hu⁴, Wentao Liang⁵, Diane Schaak¹, Eli Stavitski⁶, Jens K Nørskov^{2

7}, Samira Siahrostami^{8

9}, Haotian Wang^{10

11}

Affiliations

¹ Rowland Institute, Harvard University, Cambridge, MA, 02142, USA.
² SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
³ Center for Nanoscale Systems, Harvard University, Cambridge, MA, USA.
⁴ Canadian Light Source Inc., University of Saskatchewan, Saskatoon, SK, S7N 2V3, Canada.
⁵ Kostas Research Institute, Northeastern University, Burlington, MA, 01803, USA.
⁶ National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, 11973, USA.
⁷ SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA.
⁸ SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA. samira.siahrostami@ucalgary.ca.
⁹ Department of Chemistry, University of Calgary, 2500 University Drive NW, Calgary, Alberta, T2N 1N4, Canada. samira.siahrostami@ucalgary.ca.
¹⁰ Rowland Institute, Harvard University, Cambridge, MA, 02142, USA. htwang@rice.edu.
¹¹ Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, 77005, USA. htwang@rice.edu.

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.

Abstract

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