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dc.contributor.authorWang, Lina
dc.contributor.authorZhang, Junwei
dc.contributor.authorZheng, Lirong
dc.contributor.authorYang, Jiarui
dc.contributor.authorLi, Yongcheng
dc.contributor.authorWan, Xin
dc.contributor.authorLiu, Xiaofang
dc.contributor.authorZhang, Xixiang
dc.contributor.authorYu, Ronghai
dc.contributor.authorShui, Jianglan
dc.date.accessioned2020-07-20T12:49:57Z
dc.date.available2020-07-20T12:49:57Z
dc.date.issued2020
dc.date.submitted2020-01-31
dc.identifier.citationWang, 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
dc.identifier.issn2050-7496
dc.identifier.issn2050-7488
dc.identifier.doi10.1039/d0ta01208d
dc.identifier.urihttp://hdl.handle.net/10754/664299
dc.description.abstractCarbon 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
dc.description.sponsorshipThis work was supported by the National Natural Science Foundation of China (21673014, 21975010 and 51920105001).
dc.publisherRoyal Society of Chemistry (RSC)
dc.relation.urlhttp://xlink.rsc.org/?DOI=D0TA01208D
dc.rightsArchived with thanks to Journal of Materials Chemistry A
dc.titleCarbon black-supported FM-N-C (FM = Fe, Co, and Ni) single-atom catalysts synthesized by the self-catalysis of oxygen-coordinated ferrous metal atoms
dc.typeArticle
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.contributor.departmentMaterial Science and Engineering Program
dc.identifier.journalJournal of Materials Chemistry A
dc.rights.embargodate2021-05-29
dc.eprint.versionPost-print
dc.contributor.institutionSchool of Materials Science and Engineering, Beihang University No. 37 Xueyuan Road Beijing 100083 China
dc.contributor.institutionKey Laboratory for Magnetism and Magnetic Materials of the Ministry of Education, Lanzhou University No. 222 Tianshui Road Lanzhou 730000 China
dc.contributor.institutionBeijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences No. 19 Yuquan Road Beijing 100049 China
dc.identifier.volume8
dc.identifier.issue26
dc.identifier.pages13166-13172
kaust.personZhang, Junwei
kaust.personZhang, Xixiang
dc.date.accepted2020-5-29
dc.identifier.eid2-s2.0-85087752495
refterms.dateFOA2020-12-13T07:50:28Z


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