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

Abstract

Shifting electrochemical oxygen reduction towards 2e pathway to hydrogen peroxide (H 2O 2), instead of the traditional 4e to water, becomes increasingly important as a green method for H 2O 2 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 H 2O 2 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 H 2O 2 current, and a high H 2O 2 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 H 2O 2 pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1]; ORCiD logo [1];  [3];  [4];  [1];  [5];  [6]; ORCiD logo [7]; ORCiD logo [8]
  1. Harvard Univ., Cambridge, MA (United States)
  2. Stanford Univ., Stanford, CA (United States)
  3. Univ. of Saskatchewan, Saskatoon, SK (Canada)
  4. Northeastern Univ., Burlington, MA (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  7. Stanford Univ., Stanford, CA (United States); Univ. of Calgary, Calgary, AB (Canada)
  8. Harvard Univ., Cambridge, MA (United States); Rice Univ., Houston, TX (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1566880
Report Number(s):
BNL-212144-2019-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Jiang, Kun, Back, Seoin, Akey, Austin J., Xia, Chuan, Hu, Yongfeng, Liang, Wentao, Schaak, Diane, Stavitski, Eli, Nørskov, Jens K., Siahrostami, Samira, and Wang, Haotian. Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination. United States: N. p., 2019. Web. doi:10.1038/s41467-019-11992-2.
Jiang, Kun, Back, Seoin, Akey, Austin J., Xia, Chuan, Hu, Yongfeng, Liang, Wentao, Schaak, Diane, Stavitski, Eli, Nørskov, Jens K., Siahrostami, Samira, & Wang, Haotian. Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination. United States. doi:10.1038/s41467-019-11992-2.
Jiang, Kun, Back, Seoin, Akey, Austin J., Xia, Chuan, Hu, Yongfeng, Liang, Wentao, Schaak, Diane, Stavitski, Eli, Nørskov, Jens K., Siahrostami, Samira, and Wang, Haotian. Thu . "Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination". United States. doi:10.1038/s41467-019-11992-2. https://www.osti.gov/servlets/purl/1566880.
@article{osti_1566880,
title = {Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination},
author = {Jiang, Kun and Back, Seoin and Akey, Austin J. and Xia, Chuan and Hu, Yongfeng and Liang, Wentao and Schaak, Diane and Stavitski, Eli and Nørskov, Jens K. and Siahrostami, Samira and Wang, Haotian},
abstractNote = {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.},
doi = {10.1038/s41467-019-11992-2},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {9}
}

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