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Title: Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction

Abstract

Single-atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1–2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen-doped carbon nanotubes (MSA-N-CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA-N-CNTs, using a new multistep pyrolysis process. Among these materials, NiSA-N-CNTs show an excellent selectivity and activity for the electrochemical reduction of CO2 to CO, achieving a turnover frequency (TOF) of 11.7 s-1 at -0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.

Authors:
 [1];  [1];  [2];  [1];  [3];  [1];  [4];  [4];  [5];  [6];  [7];  [5]; ORCiD logo [1]
  1. Curtin Univ., Perth (Australia)
  2. Australian Nuclear Science and Technology Organisation (ANSTO), Melbourne, VIC (Australia). Australian Synchrotron
  3. Univ. of Western Australia, Perth, WA (Australia)
  4. Chinese Academy of Sciences (CAS), Beijing (China)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Curtin Univ., Perth (Australia); Univ. of Queensland, Brisbane (Australia); Univ. of Sunshine Coast, Maroochydore (Australia)
  7. Chinese Academy of Sciences (CAS), Beijing (China); Tsinghua Univ., Beijing (China); King Abdulaziz Univ., Jeddah (Saudi Arabia)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1543459
Alternate Identifier(s):
OSTI ID: 1419993
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 13; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Chemistry; Science & Technology - Other Topics; Materials Science; Physics

Citation Formats

Cheng, Yi, Zhao, Shiyong, Johannessen, Bernt, Veder, Jean-Pierre, Saunders, Martin, Rowles, Matthew R., Cheng, Min, Liu, Chang, Chisholm, Matthew F., De Marco, Roland, Cheng, Hui-Ming, Yang, Shi-Ze, and Jiang, San Ping. Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction. United States: N. p., 2018. Web. https://doi.org/10.1002/adma.201706287.
Cheng, Yi, Zhao, Shiyong, Johannessen, Bernt, Veder, Jean-Pierre, Saunders, Martin, Rowles, Matthew R., Cheng, Min, Liu, Chang, Chisholm, Matthew F., De Marco, Roland, Cheng, Hui-Ming, Yang, Shi-Ze, & Jiang, San Ping. Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction. United States. https://doi.org/10.1002/adma.201706287
Cheng, Yi, Zhao, Shiyong, Johannessen, Bernt, Veder, Jean-Pierre, Saunders, Martin, Rowles, Matthew R., Cheng, Min, Liu, Chang, Chisholm, Matthew F., De Marco, Roland, Cheng, Hui-Ming, Yang, Shi-Ze, and Jiang, San Ping. Fri . "Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction". United States. https://doi.org/10.1002/adma.201706287. https://www.osti.gov/servlets/purl/1543459.
@article{osti_1543459,
title = {Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction},
author = {Cheng, Yi and Zhao, Shiyong and Johannessen, Bernt and Veder, Jean-Pierre and Saunders, Martin and Rowles, Matthew R. and Cheng, Min and Liu, Chang and Chisholm, Matthew F. and De Marco, Roland and Cheng, Hui-Ming and Yang, Shi-Ze and Jiang, San Ping},
abstractNote = {Single-atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1–2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen-doped carbon nanotubes (MSA-N-CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA-N-CNTs, using a new multistep pyrolysis process. Among these materials, NiSA-N-CNTs show an excellent selectivity and activity for the electrochemical reduction of CO2 to CO, achieving a turnover frequency (TOF) of 11.7 s-1 at -0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.},
doi = {10.1002/adma.201706287},
journal = {Advanced Materials},
number = 13,
volume = 30,
place = {United States},
year = {2018},
month = {2}
}

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Cited by: 26 works
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Figures / Tables:

Figure 1 Figure 1: Characterization of NiSA-N-CNTs. A) Scanning electron microscopy (SEM) image, B) Transmission electron microscopy (TEM) image. C) STEM-EDS mapping. D) AC-STEM-annular dark field (ADF) images showing the atomic dispersion of Ni in NiSA-N-CNTs, E) ADF image showing the Ni single atoms located on the walls of a CNT (Themore » red circles show typical Ni atoms embedded in the carbon plane of walls. The insert is the Fourier transform of E). F) ADF images showing structure environment of Ni single atoms. G) Raman spectra and H) XRD patterns of NiSA-N-CNTs, Ni-N-CNTs and N-CNTs.« less

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    • DOI: 10.1039/c9se01004a

    1D/2D nitrogen-doped carbon nanorod arrays/ultrathin carbon nanosheets: outstanding catalysts for the highly efficient electroreduction of CO 2 to CO
    journal, January 2019

    • Zhu, Ying; Lv, Kuilin; Wang, Xingpu
    • Journal of Materials Chemistry A, Vol. 7, Issue 24
    • DOI: 10.1039/c9ta02353d

    N,P co-coordinated Fe species embedded in carbon hollow spheres for oxygen electrocatalysis
    journal, January 2019

    • Zhu, Xiaofeng; Tan, Xin; Wu, Kuang-Hsu
    • Journal of Materials Chemistry A, Vol. 7, Issue 24
    • DOI: 10.1039/c9ta03011e

    A copper single-atom catalyst towards efficient and durable oxygen reduction for fuel cells
    journal, January 2019

    • Cui, Liting; Cui, Lirui; Li, Zhengjian
    • Journal of Materials Chemistry A, Vol. 7, Issue 28
    • DOI: 10.1039/c9ta03518d

    Emerging nanostructured carbon-based non-precious metal electrocatalysts for selective electrochemical CO 2 reduction to CO
    journal, January 2019

    • Wang, Xinyue; Zhao, Qidong; Yang, Bin
    • Journal of Materials Chemistry A, Vol. 7, Issue 44
    • DOI: 10.1039/c9ta09681g

    Single-atom catalysts templated by metal–organic frameworks for electrochemical nitrogen reduction
    journal, January 2019

    • Zhang, Rui; Jiao, Long; Yang, Weijie
    • Journal of Materials Chemistry A, Vol. 7, Issue 46
    • DOI: 10.1039/c9ta10206j

    Effects of the Carbon Support Doping with Nitrogen for the Hydrogen Production from Formic Acid over Ni Catalysts
    journal, October 2019

    • Nishchakova, Alina D.; Bulushev, Dmitri A.; Stonkus, Olga A.
    • Energies, Vol. 12, Issue 21
    • DOI: 10.3390/en12214111

    Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn–Air Batteries
    journal, April 2021


    Enzymes Immobilized on Carbon Nitride (C 3 N 4 ) Cooperating with Metal Nanoparticles for Cascade Catalysis
    journal, January 2019

    • Wang, Yangxin; Zhang, Ningning; Hübner, René
    • Advanced Materials Interfaces, Vol. 6, Issue 6
    • DOI: 10.1002/admi.201801664

    In Situ Thermal Atomization To Convert Supported Nickel Nanoparticles into Surface-Bound Nickel Single-Atom Catalysts
    journal, October 2018

    • Yang, Jian; Qiu, Zongyang; Zhao, Changming
    • Angewandte Chemie, Vol. 130, Issue 43
    • DOI: 10.1002/ange.201808049

    Highly Efficient Electroreduction of CO 2 on Nickel Single‐Atom Catalysts: Atom Trapping and Nitrogen Anchoring
    journal, October 2019


    Heteroatom-doped carbon materials and their composites as electrocatalysts for CO 2 reduction
    journal, January 2018

    • Cui, Huijuan; Guo, Yibo; Guo, Limin
    • Journal of Materials Chemistry A, Vol. 6, Issue 39
    • DOI: 10.1039/c8ta07430e

    Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn–Air Batteries
    journal, March 2019


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.