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Currently, cation diffusion, sintering, agglomeration, and the inactivation of metal oxides during cyclic redox reactions are the key challenges hindering the widespread industrialization of the chemical looping. While encapsulation strategies using supports have shown potential for prolonging redox catalyst lifespan, the fundamental mechanisms of support\u2010redox catalyst interactions and deactivation pathways under prolonged cycling remain elusive. In this study, the varying structural evolution pathways of redox catalysts from in situ transmission electron microscopy (TEM) indicate that the SiO\n                    <jats:sub>2<\/jats:sub>\n                    shell can suppress Ostwald ripening during the reduction process through a confinement effect, thereby preventing the agglomeration of metal particles. Moreover, the activity\u2010related size\u2010dependent of Ni nanoparticles is elucidated through density functional theory (DFT) simulations. SiO\n                    <jats:sub>2<\/jats:sub>\n                    support affects the migration path during the oxidation process. Finally, redox catalysts struggle to remain stably embedded within support or securely anchored on their surfaces. The continuous separation between Ni\u2010Fe and support may serve as a critical factor in deactivation in the long\u2010term. This study offers new insights into designing hierarchical redox catalysts with enhanced thermal and redox stability through in situ observation of the actual reaction process under high\u2010temperature.\n                  <\/jats:p>","DOI":"10.1002\/smll.202503222","type":"journal-article","created":{"date-parts":[[2025,5,30]],"date-time":"2025-05-30T00:28:00Z","timestamp":1748564880000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Direct In Situ TEM Visualization of Atom Migration in SiO\n                    <sub>2<\/sub>\n                    \u2010Coated Core\u2010Shell NiFe\n                    <sub>2<\/sub>\n                    O\n                    <sub>4<\/sub>\n                    Redox Catalyst During Chemical Looping CO\n                    <sub>2<\/sub>\n                    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