From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]
Abstract
Abstract It remains highly desired but a great challenge to achieve atomically dispersed metals in high loadings for efficient catalysis. Now porphyrinic metal–organic frameworks (MOFs) have been synthesized based on a novel mixed‐ligand strategy to afford high‐content (1.76 wt %) single‐atom (SA) iron‐implanted N‐doped porous carbon (Fe SA ‐N‐C) via pyrolysis. Thanks to the single‐atom Fe sites, hierarchical pores, oriented mesochannels and high conductivity, the optimized Fe SA ‐N‐C exhibits excellent oxygen reduction activity and stability, surpassing almost all non‐noble‐metal catalysts and state‐of‐the‐art Pt/C, in both alkaline and more challenging acidic media. More far‐reaching, this MOF‐based mixed‐ligand strategy opens a novel avenue to the precise fabrication of efficient single‐atom catalysts.
- Authors:
-
- Univ. of Science and Technology of China, Anhui (People's Republic of China)
- Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chinese Academy of Sciences, Beijing (People's Republic of China)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1463675
- Alternate Identifier(s):
- OSTI ID: 1441234
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 57; Journal Issue: 28; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; metal-organic frameworks; oxygen reduction reaction; porous carbon; single-atom catalysts
Citation Formats
Jiao, Long, Wan, Gang, Zhang, Rui, Zhou, Hua, Yu, Shu -Hong, and Jiang, Hai -Long. From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]. United States: N. p., 2018.
Web. doi:10.1002/anie.201803262.
Jiao, Long, Wan, Gang, Zhang, Rui, Zhou, Hua, Yu, Shu -Hong, & Jiang, Hai -Long. From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]. United States. https://doi.org/10.1002/anie.201803262
Jiao, Long, Wan, Gang, Zhang, Rui, Zhou, Hua, Yu, Shu -Hong, and Jiang, Hai -Long. Wed .
"From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]". United States. https://doi.org/10.1002/anie.201803262. https://www.osti.gov/servlets/purl/1463675.
@article{osti_1463675,
title = {From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]},
author = {Jiao, Long and Wan, Gang and Zhang, Rui and Zhou, Hua and Yu, Shu -Hong and Jiang, Hai -Long},
abstractNote = {Abstract It remains highly desired but a great challenge to achieve atomically dispersed metals in high loadings for efficient catalysis. Now porphyrinic metal–organic frameworks (MOFs) have been synthesized based on a novel mixed‐ligand strategy to afford high‐content (1.76 wt %) single‐atom (SA) iron‐implanted N‐doped porous carbon (Fe SA ‐N‐C) via pyrolysis. Thanks to the single‐atom Fe sites, hierarchical pores, oriented mesochannels and high conductivity, the optimized Fe SA ‐N‐C exhibits excellent oxygen reduction activity and stability, surpassing almost all non‐noble‐metal catalysts and state‐of‐the‐art Pt/C, in both alkaline and more challenging acidic media. More far‐reaching, this MOF‐based mixed‐ligand strategy opens a novel avenue to the precise fabrication of efficient single‐atom catalysts.},
doi = {10.1002/anie.201803262},
journal = {Angewandte Chemie (International Edition)},
number = 28,
volume = 57,
place = {United States},
year = {Wed May 09 00:00:00 EDT 2018},
month = {Wed May 09 00:00:00 EDT 2018}
}
Web of Science
Figures / Tables:
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- Ao, Xiang; Zhang, Wei; Li, Zhishan
- Journal of Materials Chemistry A, Vol. 7, Issue 19
Mechanochemical synthesis of multi-site electrocatalysts as bifunctional zinc–air battery electrodes
journal, January 2019
- Guo, Beibei; Ju, Qiangjian; Ma, Ruguang
- Journal of Materials Chemistry A, Vol. 7, Issue 33
A review of non-precious metal single atom confined nanomaterials in different structural dimensions (1D–3D) as highly active oxygen redox reaction electrocatalysts
journal, January 2020
- Liu, Jin; Zhang, Hao; Qiu, Ming
- Journal of Materials Chemistry A, Vol. 8, Issue 5
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
Recent Advances in Isolated Single-Atom Catalysts for Zinc Air Batteries: A Focus Review
journal, October 2019
- Zhang, Weimin; Liu, Yuqing; Zhang, Lipeng
- Nanomaterials, Vol. 9, Issue 10
Migration-Prevention Strategy to Fabricate Single-Atom Fe Implanted N-Doped Porous Carbons for Efficient Oxygen Reduction
journal, August 2019
- Meng, Dong-Li; Chen, Chun-Hui; Yi, Jun-Dong
- Research, Vol. 2019
Engineering Fe–Fe 3 C@Fe–N–C Active Sites and Hybrid Structures from Dual Metal–Organic Frameworks for Oxygen Reduction Reaction in H 2 –O 2 Fuel Cell and Li–O 2 Battery
journal, April 2019
- Wang, Hao; Yin, Feng‐Xiang; Liu, Ning
- Advanced Functional Materials, Vol. 29, Issue 23
Atomic Fe‐Doped MOF‐Derived Carbon Polyhedrons with High Active‐Center Density and Ultra‐High Performance toward PEM Fuel Cells
journal, February 2019
- Deng, Yijie; Chi, Bin; Li, Jing
- Advanced Energy Materials, Vol. 9, Issue 13
Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis
journal, September 2019
- Sharifi, Tiva; Gracia‐Espino, Eduardo; Chen, Anran
- Advanced Energy Materials, Vol. 10, Issue 11
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
Encapsulating Perovskite Quantum Dots in Iron‐Based Metal–Organic Frameworks (MOFs) for Efficient Photocatalytic CO 2 Reduction
journal, July 2019
- Wu, Li‐Yuan; Mu, Yan‐Fei; Guo, Xiao‐Xuan
- Angewandte Chemie International Edition, Vol. 58, Issue 28
N‐Doped Carbon Aerogel Derived from a Metal–Organic Framework Foam as an Efficient Electrocatalyst for Oxygen Reduction
journal, July 2019
- Yi, Jun‐Dong; Zhang, Meng‐Di; Hou, Ying
- Chemistry – An Asian Journal, Vol. 14, Issue 20
Self-Sacrificial Template Synthesis of a Nitrogen-Doped Microstructured Carbon Tube as Electrocatalyst for Oxygen Reduction
journal, October 2018
- Yang, Limeng; Zeng, Yachao; Tang, Xuejun
- ChemElectroChem, Vol. 5, Issue 23
A Freestanding Flexible Single‐Atom Cobalt‐Based Multifunctional Interlayer toward Reversible and Durable Lithium‐Sulfur Batteries
journal, January 2020
- Li, Yiju; Zhou, Peng; Li, Hui
- Small Methods, Vol. 4, Issue 3
Oxygen Reduction Reactions of Fe-N-C Catalysts: Current Status and the Way Forward
journal, March 2019
- Shen, Hangjia; Thomas, Tiju; Rasaki, Sefiu Abolaji
- Electrochemical Energy Reviews, Vol. 2, Issue 2
A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
journal, August 2019
- He, Xiaohui; He, Qian; Deng, Yuchen
- Nature Communications, Vol. 10, Issue 1
A mixed-ion strategy to construct CNT-decorated Co/N-doped hollow carbon for enhanced oxygen reduction
journal, January 2018
- Feng, Taotao; Zhang, Meining
- Chemical Communications, Vol. 54, Issue 82
Interfacial proton enrichment enhances proton-coupled electrocatalytic reactions
journal, January 2018
- Zhao, Yue; Ding, Yu; Qiao, Bin
- Journal of Materials Chemistry A, Vol. 6, Issue 36
Decamethylcucurbit[5]uril based supramolecular assemblies as efficient electrocatalysts for the oxygen reduction reaction
journal, January 2019
- Chen, Ruru; Cao, Minna; Wang, Jinyun
- Chemical Communications, Vol. 55, Issue 78
Interior engineering of seaweed-derived N-doped versatile carbonaceous beads with Co x O y for universal organic pollutant degradation
journal, January 2019
- Bo, Shufeng; Zhao, Xin; An, Qingda
- RSC Advances, Vol. 9, Issue 9
Gas transport regulation in a MO/MOF interface for enhanced selective gas detection
journal, January 2019
- Yao, Ming-Shui; Cao, Lin-An; Tang, Yong-Xiang
- Journal of Materials Chemistry A, Vol. 7, Issue 31
The Challenge of Achieving a High Density of Fe-Based Active Sites in a Highly Graphitic Carbon Matrix
journal, February 2019
- Li, Jingkun; Jia, Qingying; Mukerjee, Sanjeev
- Catalysts, Vol. 9, Issue 2
A General Method for Transition Metal Single Atoms Anchored on Honeycomb‐Like Nitrogen‐Doped Carbon Nanosheets
journal, January 2020
- Zhang, Xiaoyan; Zhang, Shan; Yang, Yong
- Advanced Materials, Vol. 32, Issue 10
Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species
journal, June 2019
- Huang, Xiaoxiao; Shen, Tong; Zhang, Teng
- Advanced Energy Materials, Vol. 10, Issue 11
Atomic‐Local Environments of Single‐Atom Catalysts: Synthesis, Electronic Structure, and Activity
journal, October 2019
- Lai, Wei‐Hong; Miao, Zongcheng; Wang, Yun‐Xiao
- Advanced Energy Materials, Vol. 9, Issue 43
Promoting Frustrated Lewis Pairs for Heterogeneous Chemoselective Hydrogenation via the Tailored Pore Environment within Metal–Organic Frameworks
journal, April 2019
- Niu, Zheng; Zhang, Weijie; Lan, Pui Ching
- Angewandte Chemie, Vol. 131, Issue 22
Tailoring Nitrogen‐Doped Carbons as Hosts for Single‐Atom Catalysts
journal, May 2019
- Büchele, Simon; Chen, Zupeng; Mitchell, Sharon
- ChemCatChem, Vol. 11, Issue 12
Recent progress in pyrolyzed carbon materials as electrocatalysts for the oxygen reduction reaction
journal, January 2020
- Ouyang, Chen; Wang, Xun
- Inorganic Chemistry Frontiers, Vol. 7, Issue 1
Atomic Fe Dispersed on N-Doped Carbon Hollow Nanospheres for High-Efficiency Electrocatalytic Oxygen Reduction
journal, December 2018
- Chen, Yifan; Li, Zhijuan; Zhu, Yanbo
- Advanced Materials, Vol. 31, Issue 8
Iron Single Atoms on Graphene as Nonprecious Metal Catalysts for High‐Temperature Polymer Electrolyte Membrane Fuel Cells
journal, March 2019
- Cheng, Yi; He, Shuai; Lu, Shanfu
- Advanced Science, Vol. 6, Issue 10
Single‐Atom Cr−N 4 Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media
journal, July 2019
- Luo, Ergui; Zhang, Hao; Wang, Xian
- Angewandte Chemie, Vol. 131, Issue 36
Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation
journal, September 2019
- Pan, Yuan; Chen, Yinjuan; Wu, Konglin
- Nature Communications, Vol. 10, Issue 1
Apically Co-nanoparticles-wrapped nitrogen-doped carbon nanotubes from a single-source MOF for efficient oxygen reduction
journal, January 2018
- Ma, Lin; Wang, Rui; Li, Ya-Hui
- Journal of Materials Chemistry A, Vol. 6, Issue 47
Atomic‐ and Molecular‐Level Design of Functional Metal–Organic Frameworks (MOFs) and Derivatives for Energy and Environmental Applications
journal, August 2019
- Yilmaz, Gamze; Peh, Shing Bo; Zhao, Dan
- Advanced Science, Vol. 6, Issue 21
A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
journal, August 2019
- He, Xiaohui; He, Qian; Deng, Yuchen
- Nature Communications, Vol. 10, Issue 1
Recent Advances in Isolated Single-Atom Catalysts for Zinc Air Batteries: A Focus Review
journal, October 2019
- Zhang, Weimin; Liu, Yuqing; Zhang, Lipeng
- Nanomaterials, Vol. 9, Issue 10
Migration-Prevention Strategy to Fabricate Single-Atom Fe Implanted N-Doped Porous Carbons for Efficient Oxygen Reduction
journal, August 2019
- Meng, Dong-Li; Chen, Chun-Hui; Yi, Jun-Dong
- Research, Vol. 2019
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