Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells
Abstract
Platinum group metal (PGM)-free catalysts that are also Fe-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 vs. RHE, 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.
- Authors:
-
[3];
[7];
[5];
[4];
[10];
[11];
[2]
- Harbin Inst. of Technology (China). MIIT Key Lab. of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering; Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
- Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Oregon State Univ., Corvallis, OR (United States). School of Chemical Biological, and Environmental Engineering
- Univ. of Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Materials Science
- Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering
- Giner Inc., Newton, MA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
- Harbin Inst. of Technology (China). MIIT Key Lab. of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); Giner, Inc., Newton, MA (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1480959
- Alternate Identifier(s):
- OSTI ID: 1490583; OSTI ID: 1493892; OSTI ID: 1502572; OSTI ID: 1873085
- Report Number(s):
- BNL-209358-2018-JAAM
Journal ID: ISSN 2520-1158
- Grant/Contract Number:
- AC05-00OR22725; SC0012704; AC02-06CH11357; EE0008075
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Catalysis
- Additional Journal Information:
- Journal Volume: 1; Journal ID: ISSN 2520-1158
- Publisher:
- Springer Nature
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Chemical engineering; Electrocatalysis; Energy; Fuel cells; Heterogeneous catalysis
Citation Formats
Li, Jiazhan, Chen, Mengjie, Cullen, David A., Hwang, Sooyeon, Wang, Maoyu, Li, Boyang, Liu, Kexi, Karakalos, Stavros, Lucero, Marcos, Zhang, Hanguang, Lei, Chao, Xu, Hui, Sterbinsky, George E., Feng, Zhenxing, Su, Dong, More, Karren L., Wang, Guofeng, Wang, Zhenbo, and Wu, Gang. Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells. United States: N. p., 2018.
Web. doi:10.1038/s41929-018-0164-8.
Li, Jiazhan, Chen, Mengjie, Cullen, David A., Hwang, Sooyeon, Wang, Maoyu, Li, Boyang, Liu, Kexi, Karakalos, Stavros, Lucero, Marcos, Zhang, Hanguang, Lei, Chao, Xu, Hui, Sterbinsky, George E., Feng, Zhenxing, Su, Dong, More, Karren L., Wang, Guofeng, Wang, Zhenbo, & Wu, Gang. Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells. United States. https://doi.org/10.1038/s41929-018-0164-8
Li, Jiazhan, Chen, Mengjie, Cullen, David A., Hwang, Sooyeon, Wang, Maoyu, Li, Boyang, Liu, Kexi, Karakalos, Stavros, Lucero, Marcos, Zhang, Hanguang, Lei, Chao, Xu, Hui, Sterbinsky, George E., Feng, Zhenxing, Su, Dong, More, Karren L., Wang, Guofeng, Wang, Zhenbo, and Wu, Gang. Mon .
"Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells". United States. https://doi.org/10.1038/s41929-018-0164-8. https://www.osti.gov/servlets/purl/1480959.
@article{osti_1480959,
title = {Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells},
author = {Li, Jiazhan and Chen, Mengjie and Cullen, David A. and Hwang, Sooyeon and Wang, Maoyu and Li, Boyang and Liu, Kexi and Karakalos, Stavros and Lucero, Marcos and Zhang, Hanguang and Lei, Chao and Xu, Hui and Sterbinsky, George E. and Feng, Zhenxing and Su, Dong and More, Karren L. and Wang, Guofeng and Wang, Zhenbo and Wu, Gang},
abstractNote = {Platinum group metal (PGM)-free catalysts that are also Fe-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 vs. RHE, 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.},
doi = {10.1038/s41929-018-0164-8},
journal = {Nature Catalysis},
number = ,
volume = 1,
place = {United States},
year = {2018},
month = {10}
}
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Fig. 1: Schematic diagram of atomically dispersed MnN4 site catalyst synthesis. A two-step doping and adsorption approach can gradually increase the density of the atomically dispersed and nitrogen-coordinated MnN4 sites into the 3D carbon particles. In the first step, Mn-doped ZIF-8 precursors are carbonized and then leached with an acidmore »
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- Xiong, Xuya; Li, Yajie; Jia, Yin
- Nanoscale, Vol. 11, Issue 34
Atomic-scale engineering of MOF array confined Au nanoclusters for enhanced heterogeneous catalysis
journal, January 2019
- Gao, Ge; Xi, Qiaoyue; Zhang, Yanqun
- Nanoscale, Vol. 11, Issue 3
Atomically Dispersed Iron Cathode Catalysts Derived from Binary Ligand-Based Zeolitic Imidazolate Frameworks with Enhanced Stability for PEM Fuel Cells
journal, January 2019
- Zhang, Hanguang; Ding, Shuo; Hwang, Sooyeon
- Journal of The Electrochemical Society, Vol. 166, Issue 7
Pyridinic‐N Protected Synthesis of 3D Nitrogen‐Doped Porous Carbon with Increased Mesoporous Defects for Oxygen Reduction
journal, February 2019
- Luo, Jin; Wang, Kangjun; Hua, Xing
- Small, Vol. 15, Issue 11
Identification of Catalytic Sites for Oxygen Reduction in Metal/Nitrogen‐Doped Carbons with Encapsulated Metal Nanoparticles
journal, November 2019
- Chen, Ming‐Xi; Zhu, Mengzhao; Zuo, Ming
- Angewandte Chemie, Vol. 132, Issue 4
Zinc‐Mediated Template Synthesis of Fe‐N‐C Electrocatalysts with Densely Accessible Fe‐N x Active Sites for Efficient Oxygen Reduction
journal, January 2020
- Chen, Guangbo; Liu, Pan; Liao, Zhongquan
- Advanced Materials, Vol. 32, Issue 8
Defect‐Based Single‐Atom Electrocatalysts
journal, December 2018
- Zhang, Yiqiong; Guo, Lan; Tao, Li
- Small Methods, Vol. 3, Issue 9
Charge Transfer Modulated Activity of Carbon‐Based Electrocatalysts
journal, July 2019
- Tao, Li; Wang, Yuqing; Zou, Yuqin
- Advanced Energy Materials, Vol. 10, Issue 11
Transition Metal–Nitrogen–Carbon (M–N–C) Catalysts for Oxygen Reduction Reaction. Insights on Synthesis and Performance in Polymer Electrolyte Fuel Cells
journal, February 2019
- Osmieri, Luigi
- ChemEngineering, Vol. 3, Issue 1
Dynamic oxygen adsorption on single-atomic Ruthenium catalyst with high performance for acidic oxygen evolution reaction
journal, October 2019
- Cao, Linlin; Luo, Qiquan; Chen, Jiajia
- Nature Communications, Vol. 10, Issue 1
Identification of Catalytic Sites for Oxygen Reduction in Metal/Nitrogen‐Doped Carbons with Encapsulated Metal Nanoparticles
journal, January 2020
- Chen, Ming‐Xi; Zhu, Mengzhao; Zuo, Ming
- Angewandte Chemie International Edition, Vol. 59, Issue 4
Hierarchically porous carbons as supports for fuel cell electrocatalysts with atomically dispersed Fe–N x moieties
journal, January 2019
- Tong, Lei; Wang, Yu-Cheng; Chen, Ming-Xi
- Chemical Science, Vol. 10, Issue 35
Single‐Atomic‐Co Electrocatalysts with Self‐Supported Architecture toward Oxygen‐Involved Reaction
journal, September 2019
- Xie, Wenfu; Song, Yuke; Li, Shijin
- Advanced Functional Materials, Vol. 29, Issue 50
Volatility drivers on the metal market and exposure of producing countries
journal, August 2019
- Renner, Sven; Wellmer, Friedrich W.
- Mineral Economics, Vol. 33, Issue 3
Hierarchically Ordered Porous Carbon with Atomically Dispersed FeN 4 for Ultraefficient Oxygen Reduction Reaction in Proton‐Exchange Membrane Fuel Cells
journal, January 2020
- Qiao, Mengfei; Wang, Ying; Wang, Quan
- Angewandte Chemie, Vol. 132, Issue 7
3D porous graphitic nanocarbon for enhancing the performance and durability of Pt catalysts: a balance between graphitization and hierarchical porosity
journal, January 2019
- Qiao, Zhi; Hwang, Sooyeon; Li, Xing
- Energy & Environmental Science, Vol. 12, Issue 9
In Situ and Operando Characterization of Proton Exchange Membrane Fuel Cells
journal, August 2019
- Meyer, Quentin; Zeng, Yachao; Zhao, Chuan
- Advanced Materials, Vol. 31, Issue 40
Molecular Design of Single‐Atom Catalysts for Oxygen Reduction Reaction
journal, February 2020
- Wan, Chengzhang; Duan, Xiangfeng; Huang, Yu
- Advanced Energy Materials, Vol. 10, Issue 14
Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion
journal, November 2019
- Zhu, Yuanzhi; Sokolowski, Joshua; Song, Xiancheng
- Advanced Energy Materials, Vol. 10, Issue 11
Three-dimensional open nano-netcage electrocatalysts for efficient pH-universal overall water splitting
journal, October 2019
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- Nature Communications, Vol. 10, Issue 1
Self-templated nitrogen-doped mesoporous carbon decorated with double transition-metal active sites for enhanced oxygen electrode catalysis
journal, December 2019
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- Rare Metals, Vol. 39, Issue 7
Cobalt/zinc dual-sites coordinated with nitrogen in nanofibers enabling efficient and durable oxygen reduction reaction in acidic fuel cells
journal, January 2020
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- Journal of Materials Chemistry A, Vol. 8, Issue 7
Improving selectivity of CO reduction via reducing the coordination of critical intermediates
journal, January 2019
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- Journal of Materials Chemistry A, Vol. 7, Issue 41
Nanoporous bimetallic Zn/Fe–N–C for efficient oxygen reduction in acidic and alkaline media
journal, January 2020
- Xue, Jinling; Li, Yinshi; Hu, Jue
- Journal of Materials Chemistry A, Vol. 8, Issue 15
Atomic-level tuning of Co–N–C catalyst for high-performance electrochemical H2O2 production
journal, January 2020
- Jung, Euiyeon; Shin, Heejong; Lee, Byoung-Hoon
- Nature Materials, Vol. 19, Issue 4
Single‐Atom Cr−N 4 Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media
journal, September 2019
- Luo, Ergui; Zhang, Hao; Wang, Xian
- Angewandte Chemie International Edition, Vol. 58, Issue 36
Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN 4 Sites for Oxygen Reduction
journal, November 2019
- Li, Jiazhan; Zhang, Hanguang; Samarakoon, Widitha
- Angewandte Chemie International Edition, Vol. 58, Issue 52
A Single‐Atom Iridium Heterogeneous Catalyst in Oxygen Reduction Reaction
journal, June 2019
- Xiao, Meiling; Zhu, Jianbing; Li, Gaoran
- Angewandte Chemie, Vol. 131, Issue 28
When Nanozymes Meet Single‐Atom Catalysis
journal, October 2019
- Jiao, Lei; Yan, Hongye; Wu, Yu
- Angewandte Chemie, Vol. 132, Issue 7
Manganese acting as a high-performance heterogeneous electrocatalyst in carbon dioxide reduction
journal, July 2019
- Zhang, Bingxing; Zhang, Jianling; Shi, Jinbiao
- Nature Communications, Vol. 10, Issue 1
Three-dimensional open nano-netcage electrocatalysts for efficient pH-universal overall water splitting
journal, October 2019
- Zhuang, Zewen; Wang, Yu; Xu, Cong-Qiao
- Nature Communications, Vol. 10, Issue 1
Dynamic oxygen adsorption on single-atomic Ruthenium catalyst with high performance for acidic oxygen evolution reaction
journal, October 2019
- Cao, Linlin; Luo, Qiquan; Chen, Jiajia
- Nature Communications, Vol. 10, Issue 1
Facile Synthesis of Mayenite Electride Nanoparticles Encapsulated in Graphitic Shells Like Carbon Nano Onions: Non-noble-metal Electrocatalysts for Oxygen Reduction Reaction (ORR)
journal, January 2020
- Khan, Karim; Tareen, Ayesha Khan; Aslam, Muhammad
- Frontiers in Chemistry, Vol. 7
Recent Advances in Isolated Single-Atom Catalysts for Zinc Air Batteries: A Focus Review
journal, October 2019
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- Nanomaterials, Vol. 9, Issue 10
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