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

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

1178 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

Funding

G.Wu thanks the Research and Education in eNergy, Environment and Water (RENEW) program at the University at Buffalo, SUNY and National Science Foundation (CBET-1604392, 1804326) for partial financial support. G.Wu, G.Wang and H.X. acknowledge support from the US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office (DE-EE0008075). Electron microscopy research was conducted at Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences of (D.A.C. and K.L.M) and the Center for Functional Nanomaterials at Brookhaven National Laboratory (S.H. and D.S., under contract No. DE-SC0012704), which both are US DOE Office of Science User Facilities. XAS measurements were performed at beamline 9-BM at the Advanced Photon Source, a User Facility operated for the US DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357 (Z.F. and G.E.S.). Z.W. and J.L. thank the National Natural Science Foundation of China (Grant No. 21273058 and 21673064) for support.

Funders	Funder number
Center for Functional Nanomaterials Brookhaven National Laboratory
US Department of Energy
National Science Foundation	1804326, CBET-1604392
U.S. Department of Energy
Office of Science
Office of Energy Efficiency and Renewable Energy
Argonne National Laboratory
State University of New York
University at Buffalo
Fuel Cell Technologies Office	DE-EE0008075
National Natural Science Foundation of China	21273058, 21673064

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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

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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",

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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

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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.

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JO - Nature Catalysis

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

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