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

Jiang, Kun; Back, Seoin; Akey, Austin J.; Xia, Chuan; Hu, Yongfeng; Liang, Wentao; Schaak, Diane; Stavitski, Eli; Nørskov, Jens K.; Siahrostami, Samira; Wang, Haotian

doi:10.1038/s41467-019-11992-2

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

Journal Article · Thu Sep 05 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-11992-2· OSTI ID:1619658

;

; Akey, Austin J.;

; Hu, Yongfeng; Liang, Wentao; Schaak, Diane; Stavitski, Eli; Nørskov, Jens K.;

;

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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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: 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). Scientific User Facilities Division

Grant/Contract Number:: SC0012704; AC02-05CH11231; AC02-76SF00515; ECS-0335765; SC0008685

OSTI ID:: 1619658

Alternate ID(s):: OSTI ID: 1566880; OSTI ID: 1572051; OSTI ID: 1597946

Report Number(s):: BNL-212144-2019-JAAM; 3997; PII: 11992

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 10 Journal Issue: 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 351 works

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