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]

Jiao, Long; Wan, Gang; Zhang, Rui; Zhou, Hua; Yu, Shu -Hong; Jiang, Hai -Long

doi:10.1002/anie.201803262

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]

Journal Article · Wed May 09 00:00:00 EDT 2018 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201803262· OSTI ID:1463675

Jiao, Long ^[1]; Wan, Gang ^[2]; Zhang, Rui ^[1]; Zhou, Hua ^[3]; Yu, Shu -Hong ^[1]; Jiang, Hai -Long ^[1]

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)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1463675

Alternate ID(s):: OSTI ID: 1441234

Journal Information:: Angewandte Chemie (International Edition), Vol. 57, Issue 28; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 595 works

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Highly dispersed γ-Fe ₂ O ₃ embedded in nitrogen doped carbon for the efficient oxygen reduction reaction Xiao, Zhourong; Shen, Guoqiang; Hou, Fang Catalysis Science & Technology, Vol. 9, Issue 17 https://doi.org/10.1039/c9cy01188a	journal	January 2019
A mixed-ligand strategy regulates thorium-based MOFs Huang, Zhi-wei; Hu, Kong-qiu; Mei, Lei Dalton Transactions, Vol. 49, Issue 4 https://doi.org/10.1039/c9dt04158c	journal	January 2020
Synergistic catalysis on Fe–N _x sites and Fe nanoparticles for efficient synthesis of quinolines and quinazolinones via oxidative coupling of amines and aldehydes Ma, Zhiming; Song, Tao; Yuan, Youzhu Chemical Science, Vol. 10, Issue 44 https://doi.org/10.1039/c9sc04060a	journal	January 2019
Unraveling the high-activity nature of Fe–N–C electrocatalysts for the oxygen reduction reaction: the extraordinary synergy between Fe–N ₄ and Fe ₄ N Ao, Xiang; Zhang, Wei; Li, Zhishan Journal of Materials Chemistry A, Vol. 7, Issue 19 https://doi.org/10.1039/c9ta02338k	journal	January 2019
Mechanochemical synthesis of multi-site electrocatalysts as bifunctional zinc–air battery electrodes Guo, Beibei; Ju, Qiangjian; Ma, Ruguang Journal of Materials Chemistry A, Vol. 7, Issue 33 https://doi.org/10.1039/c9ta06411g	journal	January 2019
A review of non-precious metal single atom confined nanomaterials in different structural dimensions (1D–3D) as highly active oxygen redox reaction electrocatalysts Liu, Jin; Zhang, Hao; Qiu, Ming Journal of Materials Chemistry A, Vol. 8, Issue 5 https://doi.org/10.1039/c9ta11852g	journal	January 2020
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
Recent Advances in Isolated Single-Atom Catalysts for Zinc Air Batteries: A Focus Review Zhang, Weimin; Liu, Yuqing; Zhang, Lipeng Nanomaterials, Vol. 9, Issue 10 https://doi.org/10.3390/nano9101402	journal	October 2019
Migration-Prevention Strategy to Fabricate Single-Atom Fe Implanted N-Doped Porous Carbons for Efficient Oxygen Reduction Meng, Dong-Li; Chen, Chun-Hui; Yi, Jun-Dong Research, Vol. 2019 https://doi.org/10.34133/2019/1768595	journal	August 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 Wang, Hao; Yin, Feng‐Xiang; Liu, Ning Advanced Functional Materials, Vol. 29, Issue 23 https://doi.org/10.1002/adfm.201901531	journal	April 2019
Atomic Fe‐Doped MOF‐Derived Carbon Polyhedrons with High Active‐Center Density and Ultra‐High Performance toward PEM Fuel Cells Deng, Yijie; Chi, Bin; Li, Jing Advanced Energy Materials, Vol. 9, Issue 13 https://doi.org/10.1002/aenm.201802856	journal	February 2019
Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis Sharifi, Tiva; Gracia‐Espino, Eduardo; Chen, Anran Advanced Energy Materials, Vol. 10, Issue 11 https://doi.org/10.1002/aenm.201902084	journal	September 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
Encapsulating Perovskite Quantum Dots in Iron‐Based Metal–Organic Frameworks (MOFs) for Efficient Photocatalytic CO ₂ Reduction Wu, Li‐Yuan; Mu, Yan‐Fei; Guo, Xiao‐Xuan Angewandte Chemie International Edition, Vol. 58, Issue 28 https://doi.org/10.1002/anie.201904537	journal	July 2019
N‐Doped Carbon Aerogel Derived from a Metal–Organic Framework Foam as an Efficient Electrocatalyst for Oxygen Reduction Yi, Jun‐Dong; Zhang, Meng‐Di; Hou, Ying Chemistry – An Asian Journal, Vol. 14, Issue 20 https://doi.org/10.1002/asia.201900727	journal	July 2019
Self-Sacrificial Template Synthesis of a Nitrogen-Doped Microstructured Carbon Tube as Electrocatalyst for Oxygen Reduction Yang, Limeng; Zeng, Yachao; Tang, Xuejun ChemElectroChem, Vol. 5, Issue 23 https://doi.org/10.1002/celc.201801050	journal	October 2018
A Freestanding Flexible Single‐Atom Cobalt‐Based Multifunctional Interlayer toward Reversible and Durable Lithium‐Sulfur Batteries Li, Yiju; Zhou, Peng; Li, Hui Small Methods, Vol. 4, Issue 3 https://doi.org/10.1002/smtd.201900701	journal	January 2020
Oxygen Reduction Reactions of Fe-N-C Catalysts: Current Status and the Way Forward Shen, Hangjia; Thomas, Tiju; Rasaki, Sefiu Abolaji Electrochemical Energy Reviews, Vol. 2, Issue 2 https://doi.org/10.1007/s41918-019-00030-w	journal	March 2019
A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation He, Xiaohui; He, Qian; Deng, Yuchen Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11619-6	journal	August 2019
A mixed-ion strategy to construct CNT-decorated Co/N-doped hollow carbon for enhanced oxygen reduction Feng, Taotao; Zhang, Meining Chemical Communications, Vol. 54, Issue 82 https://doi.org/10.1039/c8cc05959d	journal	January 2018
Interfacial proton enrichment enhances proton-coupled electrocatalytic reactions Zhao, Yue; Ding, Yu; Qiao, Bin Journal of Materials Chemistry A, Vol. 6, Issue 36 https://doi.org/10.1039/c8ta06856a	journal	January 2018
Decamethylcucurbit[5]uril based supramolecular assemblies as efficient electrocatalysts for the oxygen reduction reaction Chen, Ruru; Cao, Minna; Wang, Jinyun Chemical Communications, Vol. 55, Issue 78 https://doi.org/10.1039/c9cc05899k	journal	January 2019
Interior engineering of seaweed-derived N-doped versatile carbonaceous beads with Co _x O _y for universal organic pollutant degradation Bo, Shufeng; Zhao, Xin; An, Qingda RSC Advances, Vol. 9, Issue 9 https://doi.org/10.1039/c9ra00357f	journal	January 2019
Gas transport regulation in a MO/MOF interface for enhanced selective gas detection Yao, Ming-Shui; Cao, Lin-An; Tang, Yong-Xiang Journal of Materials Chemistry A, Vol. 7, Issue 31 https://doi.org/10.1039/c9ta05226g	journal	January 2019
The Challenge of Achieving a High Density of Fe-Based Active Sites in a Highly Graphitic Carbon Matrix Li, Jingkun; Jia, Qingying; Mukerjee, Sanjeev Catalysts, Vol. 9, Issue 2 https://doi.org/10.3390/catal9020144	journal	February 2019
A General Method for Transition Metal Single Atoms Anchored on Honeycomb‐Like Nitrogen‐Doped Carbon Nanosheets Zhang, Xiaoyan; Zhang, Shan; Yang, Yong Advanced Materials, Vol. 32, Issue 10 https://doi.org/10.1002/adma.201906905	journal	January 2020
Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species Huang, Xiaoxiao; Shen, Tong; Zhang, Teng Advanced Energy Materials, Vol. 10, Issue 11 https://doi.org/10.1002/aenm.201900375	journal	June 2019
Atomic‐Local Environments of Single‐Atom Catalysts: Synthesis, Electronic Structure, and Activity Lai, Wei‐Hong; Miao, Zongcheng; Wang, Yun‐Xiao Advanced Energy Materials, Vol. 9, Issue 43 https://doi.org/10.1002/aenm.201900722	journal	October 2019
Promoting Frustrated Lewis Pairs for Heterogeneous Chemoselective Hydrogenation via the Tailored Pore Environment within Metal–Organic Frameworks Niu, Zheng; Zhang, Weijie; Lan, Pui Ching Angewandte Chemie, Vol. 131, Issue 22 https://doi.org/10.1002/ange.201903763	journal	April 2019
Tailoring Nitrogen‐Doped Carbons as Hosts for Single‐Atom Catalysts Büchele, Simon; Chen, Zupeng; Mitchell, Sharon ChemCatChem, Vol. 11, Issue 12 https://doi.org/10.1002/cctc.201900547	journal	May 2019
Recent progress in pyrolyzed carbon materials as electrocatalysts for the oxygen reduction reaction Ouyang, Chen; Wang, Xun Inorganic Chemistry Frontiers, Vol. 7, Issue 1 https://doi.org/10.1039/c9qi00962k	journal	January 2020
Atomic Fe Dispersed on N-Doped Carbon Hollow Nanospheres for High-Efficiency Electrocatalytic Oxygen Reduction Chen, Yifan; Li, Zhijuan; Zhu, Yanbo Advanced Materials, Vol. 31, Issue 8 https://doi.org/10.1002/adma.201806312	journal	December 2018
Iron Single Atoms on Graphene as Nonprecious Metal Catalysts for High‐Temperature Polymer Electrolyte Membrane Fuel Cells Cheng, Yi; He, Shuai; Lu, Shanfu Advanced Science, Vol. 6, Issue 10 https://doi.org/10.1002/advs.201802066	journal	March 2019
Single‐Atom Cr−N ₄ Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media Luo, Ergui; Zhang, Hao; Wang, Xian Angewandte Chemie, Vol. 131, Issue 36 https://doi.org/10.1002/ange.201906289	journal	July 2019
Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation Pan, Yuan; Chen, Yinjuan; Wu, Konglin Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12362-8	journal	September 2019
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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
metal-organic frameworks
oxygen reduction reaction
porous carbon
single-atom catalysts