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    Carbon black-supported FM-N-C (FM = Fe, Co, and Ni) single-atom catalysts synthesized by the self-catalysis of oxygen-coordinated ferrous metal atoms

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    Name:
    Journal of Materials Chemistry A -JL Shui.pdf
    Size:
    1.575Mb
    Format:
    PDF
    Description:
    Accepted manuscript
    Embargo End Date:
    2021-05-29
    Download
    Type
    Article
    Authors
    Wang, Lina
    Zhang, Junwei
    Zheng, Lirong cc
    Yang, Jiarui cc
    Li, Yongcheng
    Wan, Xin cc
    Liu, Xiaofang cc
    Zhang, Xixiang cc
    Yu, Ronghai
    Shui, Jianglan cc
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Material Science and Engineering Program
    Date
    2020
    Embargo End Date
    2021-05-29
    Submitted Date
    2020-01-31
    Permanent link to this record
    http://hdl.handle.net/10754/664299
    
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    Abstract
    Carbon nanomaterials have abundant sources but are difficult to use directly as a support for single atom catalysts (SACs) due to the lack of strong anchoring forces to restrict the movement and aggregation of metal atoms during the high-temperature heat treatment. Herein, we report a "self-catalysis"method for the synthesis of ferrous metal single-atom catalysts (SACs) FM-N-C (FM = Fe, Co, and Ni) with ∼2 wt% metal loadings on a carbon black support. The combination of experimental and theoretical evidence reveals a self-catalytic process from FM atoms to FM-N4 species, which involves (1) the adsorption of FM ions on the surface-oxidized carbon nanoparticles via oxygen coordination bonds (FM-O); (2) the catalytic decomposition of ammonia to nitrogen radicals on the FM atoms; (3) the replacement of coordinating oxygen with nitrogen. The precoordination of FM with oxygen is the key to the synthesis and reduces the energy barrier of ammonia decomposition and nitrogen bonding to the FM atoms. Thus, the formation of the FM-N4 species at a mild temperature of 600 °C is enabled. The as-synthesized FM-N-C SACs exhibit high catalytic activities towards O2 and/or CO2 reduction reactions. In contrast to the metal-organic framework-based SACs in which the MOF support significantly changes in size and weight, the self-catalysis technique is "minimally invasive"to the carbon support, thus benefiting the structural design of SACs by taking advantage of the abundant morphologies of the carbon nanomaterials. This journal is
    Citation
    Wang, L., Zhang, J., Zheng, L., Yang, J., Li, Y., Wan, X., … Shui, J. (2020). Carbon black-supported FM–N–C (FM = Fe, Co, and Ni) single-atom catalysts synthesized by the self-catalysis of oxygen-coordinated ferrous metal atoms. Journal of Materials Chemistry A, 8(26), 13166–13172. doi:10.1039/d0ta01208d
    Sponsors
    This work was supported by the National Natural Science Foundation of China (21673014, 21975010 and 51920105001).
    Publisher
    Royal Society of Chemistry (RSC)
    Journal
    Journal of Materials Chemistry A
    DOI
    10.1039/d0ta01208d
    Additional Links
    http://xlink.rsc.org/?DOI=D0TA01208D
    ae974a485f413a2113503eed53cd6c53
    10.1039/d0ta01208d
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Material Science and Engineering Program

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