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

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

doi:10.1038/s41929-018-0164-8

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

Journal Article · Mon Oct 29 00:00:00 EDT 2018 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-018-0164-8· OSTI ID:1480959

Li, Jiazhan ^[1]; Chen, Mengjie ^[2];

^[3]; Hwang, Sooyeon ^[4]; Wang, Maoyu ^[5]; Li, Boyang ^[6]; Liu, Kexi ^[6];

^[7]; Lucero, Marcos ^[5]; Zhang, Hanguang ^[2]; Lei, Chao ^[8]; Xu, Hui ^[8]; Sterbinsky, George E. ^[9];

^[5];

^[4];

^[10]; Wang, Guofeng ^[6];

^[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

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.

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Research Organization:: 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 Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC05-00OR22725; SC0012704; AC02-06CH11357; EE0008075

OSTI ID:: 1480959

Alternate ID(s):: OSTI ID: 1490583; OSTI ID: 1493892; OSTI ID: 1502572; OSTI ID: 1873085

Report Number(s):: BNL-209358-2018-JAAM

Journal Information:: Nature Catalysis, Vol. 1; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 806 works

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Metal–organic frameworks: a promising platform for constructing non-noble electrocatalysts for the oxygen-reduction reaction Li, Liangjun; He, Jiangxiu; Wang, Ying Journal of Materials Chemistry A, Vol. 7, Issue 5 https://doi.org/10.1039/c8ta11704g	journal	January 2019
Ultrathin atomic Mn-decorated formamide-converted N-doped carbon for efficient oxygen reduction reaction Xiong, Xuya; Li, Yajie; Jia, Yin Nanoscale, Vol. 11, Issue 34 https://doi.org/10.1039/c9nr04617h	journal	January 2019
Atomic-scale engineering of MOF array confined Au nanoclusters for enhanced heterogeneous catalysis Gao, Ge; Xi, Qiaoyue; Zhang, Yanqun Nanoscale, Vol. 11, Issue 3 https://doi.org/10.1039/c8nr07739h	journal	January 2019
Atomically Dispersed Iron Cathode Catalysts Derived from Binary Ligand-Based Zeolitic Imidazolate Frameworks with Enhanced Stability for PEM Fuel Cells Zhang, Hanguang; Ding, Shuo; Hwang, Sooyeon Journal of The Electrochemical Society, Vol. 166, Issue 7 https://doi.org/10.1149/2.0141907jes	journal	January 2019
Pyridinic‐N Protected Synthesis of 3D Nitrogen‐Doped Porous Carbon with Increased Mesoporous Defects for Oxygen Reduction Luo, Jin; Wang, Kangjun; Hua, Xing Small, Vol. 15, Issue 11 https://doi.org/10.1002/smll.201805325	journal	February 2019
Identification of Catalytic Sites for Oxygen Reduction in Metal/Nitrogen‐Doped Carbons with Encapsulated Metal Nanoparticles Chen, Ming‐Xi; Zhu, Mengzhao; Zuo, Ming Angewandte Chemie, Vol. 132, Issue 4 https://doi.org/10.1002/ange.201912275	journal	November 2019
Zinc‐Mediated Template Synthesis of Fe‐N‐C Electrocatalysts with Densely Accessible Fe‐N _x Active Sites for Efficient Oxygen Reduction Chen, Guangbo; Liu, Pan; Liao, Zhongquan Advanced Materials, Vol. 32, Issue 8 https://doi.org/10.1002/adma.201907399	journal	January 2020
Defect‐Based Single‐Atom Electrocatalysts Zhang, Yiqiong; Guo, Lan; Tao, Li Small Methods, Vol. 3, Issue 9 https://doi.org/10.1002/smtd.201800406	journal	December 2018
Charge Transfer Modulated Activity of Carbon‐Based Electrocatalysts Tao, Li; Wang, Yuqing; Zou, Yuqin Advanced Energy Materials, Vol. 10, Issue 11 https://doi.org/10.1002/aenm.201901227	journal	July 2019
Transition Metal–Nitrogen–Carbon (M–N–C) Catalysts for Oxygen Reduction Reaction. Insights on Synthesis and Performance in Polymer Electrolyte Fuel Cells Osmieri, Luigi ChemEngineering, Vol. 3, Issue 1 https://doi.org/10.3390/chemengineering3010016	journal	February 2019
Dynamic oxygen adsorption on single-atomic Ruthenium catalyst with high performance for acidic oxygen evolution reaction Cao, Linlin; Luo, Qiquan; Chen, Jiajia Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12886-z	journal	October 2019
Identification of Catalytic Sites for Oxygen Reduction in Metal/Nitrogen‐Doped Carbons with Encapsulated Metal Nanoparticles Chen, Ming‐Xi; Zhu, Mengzhao; Zuo, Ming Angewandte Chemie International Edition, Vol. 59, Issue 4 https://doi.org/10.1002/anie.201912275	journal	January 2020
Hierarchically porous carbons as supports for fuel cell electrocatalysts with atomically dispersed Fe–N _x moieties Tong, Lei; Wang, Yu-Cheng; Chen, Ming-Xi Chemical Science, Vol. 10, Issue 35 https://doi.org/10.1039/c9sc01154d	journal	January 2019
Single‐Atomic‐Co Electrocatalysts with Self‐Supported Architecture toward Oxygen‐Involved Reaction Xie, Wenfu; Song, Yuke; Li, Shijin Advanced Functional Materials, Vol. 29, Issue 50 https://doi.org/10.1002/adfm.201906477	journal	September 2019
Volatility drivers on the metal market and exposure of producing countries Renner, Sven; Wellmer, Friedrich W. Mineral Economics, Vol. 33, Issue 3 https://doi.org/10.1007/s13563-019-00200-8	journal	August 2019
Hierarchically Ordered Porous Carbon with Atomically Dispersed FeN ₄ for Ultraefficient Oxygen Reduction Reaction in Proton‐Exchange Membrane Fuel Cells Qiao, Mengfei; Wang, Ying; Wang, Quan Angewandte Chemie, Vol. 132, Issue 7 https://doi.org/10.1002/ange.201914123	journal	January 2020
3D porous graphitic nanocarbon for enhancing the performance and durability of Pt catalysts: a balance between graphitization and hierarchical porosity Qiao, Zhi; Hwang, Sooyeon; Li, Xing Energy & Environmental Science, Vol. 12, Issue 9 https://doi.org/10.1039/c9ee01899a	journal	January 2019
In Situ and Operando Characterization of Proton Exchange Membrane Fuel Cells Meyer, Quentin; Zeng, Yachao; Zhao, Chuan Advanced Materials, Vol. 31, Issue 40 https://doi.org/10.1002/adma.201901900	journal	August 2019
Molecular Design of Single‐Atom Catalysts for Oxygen Reduction Reaction Wan, Chengzhang; Duan, Xiangfeng; Huang, Yu Advanced Energy Materials, Vol. 10, Issue 14 https://doi.org/10.1002/aenm.201903815	journal	February 2020
Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion Zhu, Yuanzhi; Sokolowski, Joshua; Song, Xiancheng Advanced Energy Materials, Vol. 10, Issue 11 https://doi.org/10.1002/aenm.201902844	journal	November 2019
Three-dimensional open nano-netcage electrocatalysts for efficient pH-universal overall water splitting Zhuang, Zewen; Wang, Yu; Xu, Cong-Qiao Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12885-0	journal	October 2019
Self-templated nitrogen-doped mesoporous carbon decorated with double transition-metal active sites for enhanced oxygen electrode catalysis Qiao, Meng-Fei; Wang, Ying; Li, Lei Rare Metals, Vol. 39, Issue 7 https://doi.org/10.1007/s12598-019-01345-9	journal	December 2019
Cobalt/zinc dual-sites coordinated with nitrogen in nanofibers enabling efficient and durable oxygen reduction reaction in acidic fuel cells Zang, Jian; Wang, Feiteng; Cheng, Qingqing Journal of Materials Chemistry A, Vol. 8, Issue 7 https://doi.org/10.1039/c9ta12207a	journal	January 2020
Improving selectivity of CO reduction via reducing the coordination of critical intermediates Li, Yifan; Qian, Yumin; Ji, Yujin Journal of Materials Chemistry A, Vol. 7, Issue 41 https://doi.org/10.1039/c9ta06529f	journal	January 2019
Nanoporous bimetallic Zn/Fe–N–C for efficient oxygen reduction in acidic and alkaline media Xue, Jinling; Li, Yinshi; Hu, Jue Journal of Materials Chemistry A, Vol. 8, Issue 15 https://doi.org/10.1039/c9ta13471a	journal	January 2020
Atomic-level tuning of Co–N–C catalyst for high-performance electrochemical H2O2 production Jung, Euiyeon; Shin, Heejong; Lee, Byoung-Hoon Nature Materials, Vol. 19, Issue 4 https://doi.org/10.1038/s41563-019-0571-5	journal	January 2020
Single‐Atom Cr−N ₄ Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media Luo, Ergui; Zhang, Hao; Wang, Xian Angewandte Chemie International Edition, Vol. 58, Issue 36 https://doi.org/10.1002/anie.201906289	journal	September 2019
Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN ₄ Sites for Oxygen Reduction Li, Jiazhan; Zhang, Hanguang; Samarakoon, Widitha Angewandte Chemie International Edition, Vol. 58, Issue 52 https://doi.org/10.1002/anie.201909312	journal	November 2019
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When Nanozymes Meet Single‐Atom Catalysis Jiao, Lei; Yan, Hongye; Wu, Yu Angewandte Chemie, Vol. 132, Issue 7 https://doi.org/10.1002/ange.201905645	journal	October 2019
Facile Synthesis of Mayenite Electride Nanoparticles Encapsulated in Graphitic Shells Like Carbon Nano Onions: Non-noble-metal Electrocatalysts for Oxygen Reduction Reaction (ORR) Khan, Karim; Tareen, Ayesha Khan; Aslam, Muhammad Frontiers in Chemistry, Vol. 7 https://doi.org/10.3389/fchem.2019.00934	journal	January 2020

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25 ENERGY STORAGE
Chemical engineering
Electrocatalysis
Energy
Fuel cells
Heterogeneous catalysis