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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); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
National Science Foundation (NSF); Natural Sciences and Engineering Research Council of Canada (NSERC); National Research Council Canada; Canadian Institutes of Health Research; Province of Saskatchewan; Western Economic Diversification Canada; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1566880
Alternate Identifier(s):
OSTI ID: 1572051; OSTI ID: 1597946
Report Number(s):
BNL-212144-2019-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704; AC02-05CH11231; AC02-76SF00515; ECS-0335765; SC0008685
Resource Type:
Journal Article: 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},
issn = {2041-1723},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {9}
}

Journal Article:
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Cited by: 3 works
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Figures / Tables:

Fig. 1 Fig. 1: TEM and XAS characterizations of M-CNT catalysts. High resolution TEM and aberration-corrected HAADF-STEM images of a, e Fe-, b, f Pd-, c, g Co-, d, h Mn-CNT are shown in upper and middle panels, respectively, in which multiple rolled graphene layers can be clearly distinguished with no metalmore » clusters/particles observed in each sample. The bright dots in HAADF-STEM (marked by red arrows) represent some typical metal single atoms. Scale bars, 5 nm. il Corresponding Fourier transformed EXAFS spectra of M-CNTs are plotted in R space at the bottom panel in comparison to their bulk metal foil and metal oxide control samples« less

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