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Title: Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts

Abstract

Although single-atomically dispersed metal-Nx on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading metal-Nx is greatly challenging since the loading and single-atomic dispersion have to be balanced at high temperature for forming metal-Nx. Herein, we develop a general cascade anchoring strategy for the mass production of a series of M-NC SACs with a metal loading up to 12.1 wt%. Systematic investigation reveals that the chelation of metal ions, physical isolation of chelate complex upon high loading, and the binding with N-species at elevated temperature are essential to achieving high-loading M-NC SACs. As a demonstration, high-loading Fe-NC SAC shows superior electrocatalytic performance for O2 reduction and Ni-NC SAC exhibits high electrocatalytic activity for CO2 reduction. The strategy paves a universal way to produce stable M-NC SAC with high-density metal-Nx sites for diverse high-performance applications.

Authors:
 [1];  [2];  [1];  [3];  [4];  [1];  [1];  [5]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [4];  [4];  [4]
  1. Chinese Academy of Sciences (CAS), Beijing (China); Univ. of Chinese Academy of Sciences, Beijing (China)
  2. Chinese Academy of Sciences (CAS), Beijing (China); Sichuan Normal Univ., Chengdu (China)
  3. Univ. of Chinese Academy of Sciences, Beijing (China); Chinese Academy of Sciences (CAS), Beijing (China)
  4. Chinese Academy of Sciences (CAS), Beijing (China)
  5. Univ. of Chinese Academy of Sciences, Beijing (China); Chinese Academy of Sciences, Shanghai (China)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1559195
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhao, Lu, Zhang, Yun, Huang, Lin-Bo, Liu, Xiao-Zhi, Zhang, Qing-Hua, He, Chao, Wu, Ze-Yuan, Zhang, Lin-Juan, Wu, Jinpeng, Yang, Wanli, Gu, Lin, Hu, Jin-Song, and Wan, Li-Jun. Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts. United States: N. p., 2019. Web. doi:10.1038/s41467-019-09290-y.
Zhao, Lu, Zhang, Yun, Huang, Lin-Bo, Liu, Xiao-Zhi, Zhang, Qing-Hua, He, Chao, Wu, Ze-Yuan, Zhang, Lin-Juan, Wu, Jinpeng, Yang, Wanli, Gu, Lin, Hu, Jin-Song, & Wan, Li-Jun. Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts. United States. https://doi.org/10.1038/s41467-019-09290-y
Zhao, Lu, Zhang, Yun, Huang, Lin-Bo, Liu, Xiao-Zhi, Zhang, Qing-Hua, He, Chao, Wu, Ze-Yuan, Zhang, Lin-Juan, Wu, Jinpeng, Yang, Wanli, Gu, Lin, Hu, Jin-Song, and Wan, Li-Jun. Wed . "Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts". United States. https://doi.org/10.1038/s41467-019-09290-y. https://www.osti.gov/servlets/purl/1559195.
@article{osti_1559195,
title = {Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts},
author = {Zhao, Lu and Zhang, Yun and Huang, Lin-Bo and Liu, Xiao-Zhi and Zhang, Qing-Hua and He, Chao and Wu, Ze-Yuan and Zhang, Lin-Juan and Wu, Jinpeng and Yang, Wanli and Gu, Lin and Hu, Jin-Song and Wan, Li-Jun},
abstractNote = {Although single-atomically dispersed metal-Nx on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading metal-Nx is greatly challenging since the loading and single-atomic dispersion have to be balanced at high temperature for forming metal-Nx. Herein, we develop a general cascade anchoring strategy for the mass production of a series of M-NC SACs with a metal loading up to 12.1 wt%. Systematic investigation reveals that the chelation of metal ions, physical isolation of chelate complex upon high loading, and the binding with N-species at elevated temperature are essential to achieving high-loading M-NC SACs. As a demonstration, high-loading Fe-NC SAC shows superior electrocatalytic performance for O2 reduction and Ni-NC SAC exhibits high electrocatalytic activity for CO2 reduction. The strategy paves a universal way to produce stable M-NC SAC with high-density metal-Nx sites for diverse high-performance applications.},
doi = {10.1038/s41467-019-09290-y},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Wed Mar 20 00:00:00 EDT 2019},
month = {Wed Mar 20 00:00:00 EDT 2019}
}

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Single Atom (Pd/Pt) Supported on Graphitic Carbon Nitride as an Efficient Photocatalyst for Visible-Light Reduction of Carbon Dioxide
journal, May 2016

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Uncoordinated Amine Groups of Metal–Organic Frameworks to Anchor Single Ru Sites as Chemoselective Catalysts toward the Hydrogenation of Quinoline
journal, July 2017

  • Wang, Xin; Chen, Wenxing; Zhang, Lei
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  • DOI: 10.1021/jacs.7b01686

Photodegradation Performance of g-C 3 N 4 Fabricated by Directly Heating Melamine
journal, September 2009

  • Yan, S. C.; Li, Z. S.; Zou, Z. G.
  • Langmuir, Vol. 25, Issue 17
  • DOI: 10.1021/la900923z

Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts
journal, November 2017

  • Shan, Junjun; Li, Mengwei; Allard, Lawrence F.
  • Nature, Vol. 551, Issue 7682
  • DOI: 10.1038/nature24640

Single-atom catalysis of CO oxidation using Pt1/FeOx
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Platinum single-atom and cluster catalysis of the hydrogen evolution reaction
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High performance platinum single atom electrocatalyst for oxygen reduction reaction
journal, July 2017

  • Liu, Jing; Jiao, Menggai; Lu, Lanlu
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15938

Promotion of oxygen reduction by a bio-inspired tethered iron phthalocyanine carbon nanotube-based catalyst
journal, June 2013

  • Cao, Ruiguo; Thapa, Ranjit; Kim, Hyejung
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3076

Atomic cobalt on nitrogen-doped graphene for hydrogen generation
journal, October 2015

  • Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9668

Subnanometre platinum clusters as highly active and selective catalysts for the oxidative dehydrogenation of propane
journal, February 2009

  • Vajda, Stefan; Pellin, Michael J.; Greeley, Jeffrey P.
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