General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities

Fei, Huilong; Dong, Juncai; Feng, Yexin; Allen, Christopher S.; Wan, Chengzhang; Volosskiy, Boris; Li, Mufan; Zhao, Zipeng; Wang, Yiliu; Sun, Hongtao; An, Pengfei; Chen, Wenxing; Guo, Zhiying; Lee, Chain; Chen, Dongliang; Shakir, Imran; Liu, Mingjie; Hu, Tiandou; Li, Yadong; Kirkland, Angus I.; Duan, Xiangfeng; Huang, Yu

doi:10.1038/s41929-017-0008-y

Title: General synthesis and definitive structural identification of MN₄C₄ single-atom catalysts with tunable electrocatalytic activities

Journal Article · Mon Jan 08 00:00:00 EST 2018 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-017-0008-y· OSTI ID:1425042

Fei, Huilong ^[1];

^[2]; Feng, Yexin ^[3];

^[4]; Wan, Chengzhang ^[1]; Volosskiy, Boris ^[1]; Li, Mufan ^[1]; Zhao, Zipeng ^[1]; Wang, Yiliu ^[1];

^[1]; An, Pengfei ^[2];

^[5]; Guo, Zhiying ^[2]; Lee, Chain ^[1]; Chen, Dongliang ^[2]; Shakir, Imran ^[6]; Liu, Mingjie ^[7]; Hu, Tiandou ^[2]; Li, Yadong ^[5]; Kirkland, Angus I. ^[4] more »

Univ. of California, Los Angeles, CA (United States)
Chinese Academy of Sciences (CAS), Beijing (China)
Hunan Univ., Changsha (China)
Univ. of Oxford (United Kingdom); Science and Technology Facilities Council (STFC), Harwell Campus, Oxford (United Kingdom). Diamond Light Source, Ltd.
Tsinghua Univ., Beijing (China)
King Saud Univ., Riyadh (Saudi Arabia)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Single-atom catalysts (SACs) have recently attracted broad research interest as they combine the merits of both homogeneous and heterogeneous catalysts. Rational design and synthesis of SACs are of immense significance but have so far been plagued by the lack of a definitive correlation between structure and catalytic properties. Here, we report a general approach to a series of monodispersed atomic transition metals (for example, Fe, Co, Ni) embedded in nitrogen-doped graphene with a common MNsub>4C₄ moiety, identified by systematic X-ray absorption fine structure analyses and direct transmission electron microscopy imaging. The unambiguous structure determination allows density functional theoretical prediction of MNsub>4C₄ moieties as efficient oxygen evolution catalysts with activities following the trend Ni > Co > Fe, which is confirmed by electrochemical measurements. Determination of atomistic structure and its correlation with catalytic properties represents a critical step towards the rational design and synthesis of precious or nonprecious SACs with exceptional atom utilization efficiency and catalytic activities.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1425042

Report Number(s):: BNL-200041-2018-JAAM

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

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 1216 works

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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
Manganese acting as a high-performance heterogeneous electrocatalyst in carbon dioxide reduction Zhang, Bingxing; Zhang, Jianling; Shi, Jinbiao Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10854-1	journal	July 2019
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Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions Yan, Xiao; Liu, Daolan; Cao, Huanhuan Small Methods, Vol. 3, Issue 9 https://doi.org/10.1002/smtd.201800501	journal	February 2019
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Electrochemical deposition as a universal route for fabricating single-atom catalysts Zhang, Zhirong; Feng, Chen; Liu, Chunxiao Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-14917-6	journal	March 2020
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Insights into Single‐Atom Metal–Support Interactions in Electrocatalytic Water Splitting Zhang, Jingfang; Liu, Cuibo; Zhang, Bin Small Methods, Vol. 3, Issue 9 https://doi.org/10.1002/smtd.201800481	journal	February 2019
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Catalysis of a Single Transition Metal Site for Water Oxidation: From Mononuclear Molecules to Single Atoms Zhang, Huayang; Tian, Wenjie; Duan, Xiaoguang Advanced Materials, Vol. 32, Issue 18 https://doi.org/10.1002/adma.201904037	journal	December 2019
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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
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Modulierung der elektronischen Strukturen anorganischer Nanomaterialien für eine effiziente elektrokatalytische Wasserspaltung Du, Xinchuan; Huang, Jianwen; Zhang, Junjun Angewandte Chemie, Vol. 131, Issue 14 https://doi.org/10.1002/ange.201810104	journal	February 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
Atomically dispersed nickel–nitrogen–sulfur species anchored on porous carbon nanosheets for efficient water oxidation Hou, Yang; Qiu, Ming; Kim, Min Gyu Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09394-5	journal	March 2019
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
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
Transition metal embedded C ₃ N monolayers as promising catalysts for the hydrogen evolution reaction Zhao, Yameng; Ma, Dongwei; Zhang, Jing Physical Chemistry Chemical Physics, Vol. 21, Issue 36 https://doi.org/10.1039/c9cp04267a	journal	January 2019
Recent Progress in Defective Carbon‐Based Oxygen Electrode Materials for Rechargeable Zink‐Air Batteries Wang, Sidi; Jiang, Hongliang; Song, Li Batteries & Supercaps, Vol. 2, Issue 6 https://doi.org/10.1002/batt.201900001	journal	April 2019
Multiscale carbon foam confining single iron atoms for efficient electrocatalytic CO2 reduction to CO Zhang, Zheng; Ma, Chao; Tu, Yunchuan Nano Research, Vol. 12, Issue 9 https://doi.org/10.1007/s12274-019-2316-9	journal	March 2019
Metal single-atom coordinated graphitic carbon nitride as an efficient catalyst for CO oxidation Wang, Shiyan; Li, Jiaqi; Li, Qiang Nanoscale, Vol. 12, Issue 1 https://doi.org/10.1039/c9nr07726j	journal	January 2020
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
Confinement Catalysis with 2D Materials for Energy Conversion Tang, Lei; Meng, Xianguang; Deng, Dehui Advanced Materials, Vol. 31, Issue 50 https://doi.org/10.1002/adma.201901996	journal	July 2019

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