Nitrogen-Coordinated Single Cobalt Atom Catalysts for Oxygen Reduction in Proton Exchange Membrane Fuel Cells

Wang, Xiao Xia; Cullen, David A.; Pan, Yung-Tin; Hwang, Sooyeon; Wang, Maoyu; Feng, Zhenxing; Wang, Jingyun; Engelhard, Mark H.; Zhang, Hanguang; He, Yanghua; Shao, Yuyan; Su, Dong; More, Karren L.; Spendelow, Jacob S.; Wu, Gang

doi:10.1002/adma.201706758

Title: Nitrogen-Coordinated Single Cobalt Atom Catalysts for Oxygen Reduction in Proton Exchange Membrane Fuel Cells

Journal Article · 24 January 2018 · Advanced Materials

DOI: https://doi.org/10.1002/adma.201706758 · OSTI ID:1422592

Wang, Xiao Xia ^[1]; Cullen, David A. ^[2]; Pan, Yung-Tin ^[3]; Hwang, Sooyeon ^[4]; Wang, Maoyu ^[5]; Feng, Zhenxing ^[5]; Wang, Jingyun ^[6]; Engelhard, Mark H. ^[7]; Zhang, Hanguang ^[6]; He, Yanghua ^[6]; Shao, Yuyan ^[7]; Su, Dong ^[4]; More, Karren L. ^[8]; Spendelow, Jacob S. ^[3];

^[6]

Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering; East China Univ. of Science and Technology, Shanghai (China). School of Mechanical and Power Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Oregon State Univ., Corvallis, OR (United States). School of Chemical, Biological, and Environmental Engineering
Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences

Due to the Fenton reaction, the presence of Fe and peroxide in electrodes generates free radicals causing serious degradation of the organic ionomer and the membrane. Pt-free and Fe-free cathode catalysts therefore are urgently needed for durable and inexpensive proton exchange membrane fuel cells (PEMFCs). In this paper, a high-performance nitrogen-coordinated single Co atom catalyst is derived from Co-doped metal-organic frameworks (MOFs) through a one-step thermal activation. Aberration-corrected electron microscopy combined with X-ray absorption spectroscopy virtually verifies the CoN₄ coordination at an atomic level in the catalysts. Through investigating effects of Co doping contents and thermal activation temperature, an atomically Co site dispersed catalyst with optimal chemical and structural properties has achieved respectable activity and stability for the oxygen reduction reaction (ORR) in challenging acidic media (e.g., half-wave potential of 0.80 V vs reversible hydrogen electrode (RHE). The performance is comparable to Fe-based catalysts and 60 mV lower than Pt/C -60 μg Pt cm^-2). Fuel cell tests confirm that catalyst activity and stability can translate to high-performance cathodes in PEMFCs. Finally, the remarkably enhanced ORR performance is attributed to the presence of well-dispersed CoN₄ active sites embedded in 3D porous MOF-derived carbon particles, omitting any inactive Co aggregates.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Univ. at Buffalo, NY (United States); East China Univ. of Science and Technology, Shanghai (China); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation and Fuels. Hydrogen and Fuel Cell Technologies Office (HFTO); USDOE Office of Science (SC); National Science Foundation (NSF); Shanghai Natural Science Foundation of China; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357; SC0012704; CBET-1604392; 16ZR1408600; 89233218CNA000001

OSTI ID:: 1422592

Alternate ID(s):: OSTI ID: 1417922; OSTI ID: 1558078

Report Number(s):: LA-UR-19-27321; TRN: US1801631

Journal Information:: Advanced Materials, Vol. 30, Issue 11; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Dispersive Single-Atom Metals Anchored on Functionalized Nanocarbons for Electrochemical Reactions Li, Jin-Cheng; Wei, Zidong; Liu, Dong Topics in Current Chemistry, Vol. 377, Issue 1 https://doi.org/10.1007/s41061-018-0229-9	journal	January 2019
Controllable synthesis of CoN ₃ catalysts derived from Co/Zn-ZIF-67 for electrocatalytic oxygen reduction in acidic electrolytes Lai, Shoujuan; Xu, Li; Liu, Hongli Journal of Materials Chemistry A, Vol. 7, Issue 38 https://doi.org/10.1039/c9ta08134h	journal	January 2019
The Multifaceted Reactivity of Single-Atom Heterogeneous Catalysts Mitchell, Sharon; Vorobyeva, Evgeniya; Pérez-Ramírez, Javier Angewandte Chemie International Edition, Vol. 57, Issue 47 https://doi.org/10.1002/anie.201806936	journal	October 2018
Atomically Dispersed Binary Co‐Ni Sites in Nitrogen‐Doped Hollow Carbon Nanocubes for Reversible Oxygen Reduction and Evolution Han, Xiaopeng; Ling, Xiaofei; Yu, Deshuang Advanced Materials, Vol. 31, Issue 49 https://doi.org/10.1002/adma.201905622	journal	October 2019
Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N ₂ and H ₂ O Mukherjee, Shreya; Yang, Xiaoxuan; Shan, Weitao Small Methods, Vol. 4, Issue 6 https://doi.org/10.1002/smtd.201900821	journal	February 2020
Fe–N–C electrocatalyst with dense active sites and efficient mass transport for high-performance proton exchange membrane fuel cells Wan, Xin; Liu, Xiaofang; Li, Yongcheng Nature Catalysis, Vol. 2, Issue 3 https://doi.org/10.1038/s41929-019-0237-3	journal	March 2019
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Carbon-Rich Nanomaterials: Fascinating Hydrogen and Oxygen Electrocatalysts Zhang, Jian; Chen, Guangbo; Müllen, Klaus Advanced Materials, Vol. 30, Issue 40 https://doi.org/10.1002/adma.201800528	journal	July 2018
Unveiling the Activity Origin of Electrocatalytic Oxygen Evolution over Isolated Ni Atoms Supported on a N‐Doped Carbon Matrix Zhang, Huabin; Liu, Yanyu; Chen, Tao Advanced Materials, Vol. 31, Issue 48 https://doi.org/10.1002/adma.201904548	journal	October 2019
Two‐Dimensional Conjugated Aromatic Networks as High‐Site‐Density and Single‐Atom Electrocatalysts for the Oxygen Reduction Reaction Yang, Shaoxuan; Yu, Yihuan; Dou, Meiling Angewandte Chemie International Edition, Vol. 58, Issue 41 https://doi.org/10.1002/anie.201908023	journal	September 2019
Rapid and energy-efficient microwave pyrolysis for high-yield production of highly-active bifunctional electrocatalysts for water splitting Huang, Huawei; Zhou, Si; Yu, Chang Energy & Environmental Science, Vol. 13, Issue 2 https://doi.org/10.1039/c9ee03273h	journal	January 2020
Cobalt‐based coordination polymer as high activity electrocatalyst for oxygen reduction reaction: Catalysis by novel active site CoO ₄ N ₂ Chen, Xin; Ge, Fan; Lai, Nanjun International Journal of Energy Research, Vol. 44, Issue 3 https://doi.org/10.1002/er.5074	journal	December 2019
Carbon‐Based Metal‐Free ORR Electrocatalysts for Fuel Cells: Past, Present, and Future Yang, Lijun; Shui, Jianglan; Du, Lei Advanced Materials, Vol. 31, Issue 13 https://doi.org/10.1002/adma.201804799	journal	January 2019
Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN ₄ Sites for Oxygen Reduction Li, Jiazhan; Zhang, Hanguang; Samarakoon, Widitha Angewandte Chemie, Vol. 131, Issue 52 https://doi.org/10.1002/ange.201909312	journal	November 2019
Atomic‐Scale Insights into the Low‐Temperature Oxidation of Methanol over a Single‐Atom Pt ₁ ‐Co ₃ O ₄ Catalyst Jiang, Zeyu; Feng, Xiangbo; Deng, Jianlin Advanced Functional Materials, Vol. 29, Issue 31 https://doi.org/10.1002/adfm.201902041	journal	April 2019
Cobalt Nanoparticles and Atomic Sites in Nitrogen‐Doped Carbon Frameworks for Highly Sensitive Sensing of Hydrogen Peroxide Li, Zehui; Liu, Rongji; Tang, Cheng Small, Vol. 16, Issue 15 https://doi.org/10.1002/smll.201902860	journal	August 2019
Preparation of reduced graphite oxide loaded with cobalt(II) and nitrogen co-doped carbon polyhedrons from a metal-organic framework (type ZIF-67), and its application to electrochemical determination of metronidazole Chen, Han; Wu, Xingxing; Zhao, Rui Microchimica Acta, Vol. 186, Issue 9 https://doi.org/10.1007/s00604-019-3737-6	journal	August 2019
Metal-Nitrogen-Carbon Catalysts for Oxygen Reduction in PEM Fuel Cells: Self-Template Synthesis Approach to Enhancing Catalytic Activity and Stability He, Yanghua; Tan, Qiang; Lu, Leilei Electrochemical Energy Reviews, Vol. 2, Issue 2 https://doi.org/10.1007/s41918-019-00031-9	journal	March 2019
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Ultrathin‐Carbon‐Layer‐Protected PtCu Nanoparticles Encapsulated in Carbon Capsules: A Structure Engineering of the Anode Electrocatalyst for Direct Formic Acid Fuel Cells Xu, Min; Chen, Hong; Zhao, Yufei Particle & Particle Systems Characterization, Vol. 36, Issue 7 https://doi.org/10.1002/ppsc.201900100	journal	May 2019
Core-Shell Polydopamine@Zr-Hemin MOFs Derived Fe-N-Doped Porous Carbon Nanospheres Electrocatalysts for the Oxygen Reduction Wang, Yinling; Wang, Juan; Zhang, Youliang Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.1101810jes	journal	January 2018
Direct fabrication of bimetallic AuPt nanobrick spherical nanoarchitectonics for the oxygen reduction reaction Narendra Kumar, Alam Venugopal; Yin, Shuli; Wang, Ziqiang New Journal of Chemistry, Vol. 43, Issue 24 https://doi.org/10.1039/c9nj01983a	journal	January 2019
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Bacterium, Fungus, and Virus Microorganisms for Energy Storage and Conversion Shen, Shenghui; Zhou, Rongfan; Li, Yahao Small Methods, Vol. 3, Issue 12 https://doi.org/10.1002/smtd.201900596	journal	October 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
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Single and double boron atoms doped nanoporous C ₂ N– h 2D electrocatalysts for highly efficient N ₂ reduction reaction: a density functional theory study Cao, Yongyong; Deng, Shengwei; Fang, Qiaojun Nanotechnology, Vol. 30, Issue 33 https://doi.org/10.1088/1361-6528/ab1d01	journal	May 2019
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Iron‐Free Cathode Catalysts for Proton‐Exchange‐Membrane Fuel Cells: Cobalt Catalysts and the Peroxide Mitigation Approach Wang, Xiao Xia; Prabhakaran, Venkateshkumar; He, Yanghua Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201805126	journal	December 2018
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Carbon-Supported Single Atom Catalysts for Electrochemical Energy Conversion and Storage Peng, Yi; Lu, Bingzhang; Chen, Shaowei Advanced Materials, Vol. 30, Issue 48 https://doi.org/10.1002/adma.201801995	journal	August 2018
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The simplest construction of single-site catalysts by the synergism of micropore trapping and nitrogen anchoring Zhang, Zhiqi; Chen, Yugang; Zhou, Liqi Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09596-x	journal	April 2019
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Fe-doped mayenite electride composite with 2D reduced Graphene Oxide: As a non-platinum based, highly durable electrocatalyst for Oxygen Reduction Reaction Khan, Karim; Tareen, Ayesha Khan; Aslam, Muhammad Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-55207-6	journal	December 2019
Novel Two-Dimensional Carbon–Chromium Nitride-Based Composite as an Electrocatalyst for Oxygen Reduction Reaction Khan, Karim; Tareen, Ayesha Khan; Aslam, Muhammad Frontiers in Chemistry, Vol. 7 https://doi.org/10.3389/fchem.2019.00738	journal	November 2019
Alloyed Pt ₃ M (M = Co, Ni) nanoparticles supported on S- and N-doped carbon nanotubes for the oxygen reduction reaction Louisia, Stéphane; Thomas, Yohann R. J.; Lecante, Pierre Beilstein Journal of Nanotechnology, Vol. 10 https://doi.org/10.3762/bjnano.10.125	journal	January 2019

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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