Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells

Jiazhan Li; Mengjie Chen; David A. Cullen; Sooyeon Hwang; Maoyu Wang; Boyang Li; Kexi Liu; Stavros Karakalos; Marcos Lucero; Hanguang Zhang; Chao Lei; Hui Xu; George E. Sterbinsky; Zhenxing Feng; Dong Su; Karren L. More; Guofeng Wang; Zhenbo Wang; Gang Wu

doi:10.1038/s41929-018-0164-8

Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells

Jiazhan Li
, Mengjie Chen
, David A. Cullen
, Sooyeon Hwang
, Maoyu Wang
, Boyang Li
, Kexi Liu
, Stavros Karakalos
, Marcos Lucero
, Hanguang Zhang
, Chao Lei
, Hui Xu
, George E. Sterbinsky
, Zhenxing Feng
, Dong Su
, Karren L. More
, Guofeng Wang
, Zhenbo Wang
, Gang Wu

Department of Chemical and Biological Engineering

Harbin Institute of Technology
SUNY Buffalo
Oak Ridge National Laboratory
Brookhaven National Laboratory
Oregon State University
University of Pittsburgh
University of South Carolina
Giner, Incorporated and Giner Electrochemical Systems, LLC
United States Department of Energy

Research output: Contribution to journal › Article › peer-review

1394 Scopus citations

Abstract

Platinum group metal (PGM)-free catalysts that are also iron free are highly desirable for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells, as they avoid possible Fenton reactions. Here we report an efficient ORR catalyst that consists of atomically dispersed nitrogen-coordinated single Mn sites on partially graphitic carbon (Mn-N-C). Evidence for the embedding of the atomically dispersed MnN₄ moieties within the carbon surface-exposed basal planes was established by X-ray absorption spectroscopy and their dispersion was confirmed by aberration-corrected electron microscopy with atomic resolution. The Mn-N-C catalyst exhibited a half-wave potential of 0.80 V versus the reversible hydrogen electrode, approaching that of Fe-N-C catalysts, along with significantly enhanced stability in acidic media. The encouraging performance of the Mn-N-C catalyst as a PGM-free cathode was demonstrated in fuel cell tests. First-principles calculations further support the MnN₄ sites as the origin of the ORR activity via a 4e⁻ pathway in acidic media.

Original language	English
Pages (from-to)	935-945
Number of pages	11
Journal	Nature Catalysis
Volume	1
Issue number	12
DOIs	https://doi.org/10.1038/s41929-018-0164-8
State	Published - Dec 1 2018

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Li, J., Chen, M., Cullen, D. A., Hwang, S., Wang, M., Li, B., Liu, K., Karakalos, S., Lucero, M., Zhang, H., Lei, C., Xu, H., Sterbinsky, G. E., Feng, Z., Su, D., More, K. L., Wang, G., Wang, Z., & Wu, G. (2018). Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells. Nature Catalysis, 1(12), 935-945. https://doi.org/10.1038/s41929-018-0164-8

@article{010e8281b7574366a10eaeb0bc4ece9f,

title = "Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells",

abstract = "Platinum group metal (PGM)-free catalysts that are also iron free are highly desirable for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells, as they avoid possible Fenton reactions. Here we report an efficient ORR catalyst that consists of atomically dispersed nitrogen-coordinated single Mn sites on partially graphitic carbon (Mn-N-C). Evidence for the embedding of the atomically dispersed MnN4 moieties within the carbon surface-exposed basal planes was established by X-ray absorption spectroscopy and their dispersion was confirmed by aberration-corrected electron microscopy with atomic resolution. The Mn-N-C catalyst exhibited a half-wave potential of 0.80 V versus the reversible hydrogen electrode, approaching that of Fe-N-C catalysts, along with significantly enhanced stability in acidic media. The encouraging performance of the Mn-N-C catalyst as a PGM-free cathode was demonstrated in fuel cell tests. First-principles calculations further support the MnN4 sites as the origin of the ORR activity via a 4e− pathway in acidic media.",

author = "Jiazhan Li and Mengjie Chen and Cullen, \{David A.\} and Sooyeon Hwang and Maoyu Wang and Boyang Li and Kexi Liu and Stavros Karakalos and Marcos Lucero and Hanguang Zhang and Chao Lei and Hui Xu and Sterbinsky, \{George E.\} and Zhenxing Feng and Dong Su and More, \{Karren L.\} and Guofeng Wang and Zhenbo Wang and Gang Wu",

note = "Publisher Copyright: {\textcopyright} 2018, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2018",

month = dec,

day = "1",

doi = "10.1038/s41929-018-0164-8",

language = "English",

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Li, J, Chen, M, Cullen, DA, Hwang, S, Wang, M, Li, B, Liu, K, Karakalos, S, Lucero, M, Zhang, H, Lei, C, Xu, H, Sterbinsky, GE, Feng, Z, Su, D, More, KL, Wang, G, Wang, Z & Wu, G 2018, 'Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells', Nature Catalysis, vol. 1, no. 12, pp. 935-945. https://doi.org/10.1038/s41929-018-0164-8

TY - JOUR

T1 - Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells

AU - Li, Jiazhan

AU - Chen, Mengjie

AU - Cullen, David A.

AU - Hwang, Sooyeon

AU - Wang, Maoyu

AU - Li, Boyang

AU - Liu, Kexi

AU - Karakalos, Stavros

AU - Lucero, Marcos

AU - Zhang, Hanguang

AU - Lei, Chao

AU - Xu, Hui

AU - Sterbinsky, George E.

AU - Feng, Zhenxing

AU - Su, Dong

AU - More, Karren L.

AU - Wang, Guofeng

AU - Wang, Zhenbo

AU - Wu, Gang

PY - 2018/12/1

Y1 - 2018/12/1

N2 - Platinum group metal (PGM)-free catalysts that are also iron free are highly desirable for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells, as they avoid possible Fenton reactions. Here we report an efficient ORR catalyst that consists of atomically dispersed nitrogen-coordinated single Mn sites on partially graphitic carbon (Mn-N-C). Evidence for the embedding of the atomically dispersed MnN4 moieties within the carbon surface-exposed basal planes was established by X-ray absorption spectroscopy and their dispersion was confirmed by aberration-corrected electron microscopy with atomic resolution. The Mn-N-C catalyst exhibited a half-wave potential of 0.80 V versus the reversible hydrogen electrode, approaching that of Fe-N-C catalysts, along with significantly enhanced stability in acidic media. The encouraging performance of the Mn-N-C catalyst as a PGM-free cathode was demonstrated in fuel cell tests. First-principles calculations further support the MnN4 sites as the origin of the ORR activity via a 4e− pathway in acidic media.

AB - Platinum group metal (PGM)-free catalysts that are also iron free are highly desirable for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells, as they avoid possible Fenton reactions. Here we report an efficient ORR catalyst that consists of atomically dispersed nitrogen-coordinated single Mn sites on partially graphitic carbon (Mn-N-C). Evidence for the embedding of the atomically dispersed MnN4 moieties within the carbon surface-exposed basal planes was established by X-ray absorption spectroscopy and their dispersion was confirmed by aberration-corrected electron microscopy with atomic resolution. The Mn-N-C catalyst exhibited a half-wave potential of 0.80 V versus the reversible hydrogen electrode, approaching that of Fe-N-C catalysts, along with significantly enhanced stability in acidic media. The encouraging performance of the Mn-N-C catalyst as a PGM-free cathode was demonstrated in fuel cell tests. First-principles calculations further support the MnN4 sites as the origin of the ORR activity via a 4e− pathway in acidic media.

UR - https://www.scopus.com/pages/publications/85055699589

U2 - 10.1038/s41929-018-0164-8

DO - 10.1038/s41929-018-0164-8

M3 - Article

AN - SCOPUS:85055699589

SN - 2520-1158

VL - 1

SP - 935

EP - 945

JO - Nature Catalysis

JF - Nature Catalysis

IS - 12

ER -

Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells

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