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Herein, the authors record the complete evolution process of Co SAC during the pyrolysis a Co\/Zn\u2010containing zeolitic imidazolate framework. Aberration\u2010corrected environmental TEM coupled with in\u2010situ EELS is used for direct visualization of the evolution process at 200\u20131000\u00a0\u00b0C. Dissolution of carbon into the nanoparticles of Co is found to be key to modulating the wetting behavior of nanoparticles on the carbon support; melting of Co nanoparticles and their motion within the zeolitic architecture leads to the etching of the framework structure, yielding porous C\/N support onto which Co\u2010single atoms reside. This uniquely structured Co SAC is found to be effective for the oxidation of a series of aromatic alkanes to produce selective ketones among other possible products. The carbon dissolution and melting\/sublimation\u2010driven structural dynamics of transition metal revealed here will expand the methodology in synthesizing SACs and other high\u2010temperature processes.<\/jats:p>","DOI":"10.1002\/advs.202200592","type":"journal-article","created":{"date-parts":[[2022,5,4]],"date-time":"2022-05-04T22:25:11Z","timestamp":1651703111000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":38,"title":["Direct Visualization of the Evolution of a Single\u2010Atomic Cobalt Catalyst from Melting Nanoparticles with Carbon Dissolution"],"prefix":"10.1002","volume":"9","author":[{"given":"Luyao","family":"Zhang","sequence":"first","affiliation":[{"name":"Department of Chemistry Guangdong Provincial Key Laboratory of Catalysis Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Key Laboratory of Energy Conversion and Storage Technologies (Ministry of Education) Southern University of 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