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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Journal of Materials Chemistry A -JL Shui.pdf
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2021-05-29
Type
ArticleAuthors
Wang, LinaZhang, Junwei
Zheng, Lirong

Yang, Jiarui

Li, Yongcheng
Wan, Xin

Liu, Xiaofang

Zhang, Xixiang

Yu, Ronghai
Shui, Jianglan

KAUST Department
Physical Science and Engineering (PSE) DivisionMaterial Science and Engineering Program
Date
2020Embargo End Date
2021-05-29Submitted Date
2020-01-31Permanent link to this record
http://hdl.handle.net/10754/664299
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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 isCitation
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/d0ta01208dSponsors
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 AAdditional Links
http://xlink.rsc.org/?DOI=D0TA01208Dae974a485f413a2113503eed53cd6c53
10.1039/d0ta01208d