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Conventional catalyst sintering theory largely ignores the entropy effect and suggests that ADCs are normally thermodynamically unstable due to their high surface free energies, which becomes an obstacle for practical applications. Here, we present a generalized thermodynamic framework to demonstrate how the previously ignored entropy effect induces the self-redispersion of supported NPs. Through machine-learning-assisted molecular dynamics simulations, in situ Cs-corrected environmental scanning transmission electron microscopy, and synchrotron-based ambient-pressure X-ray photoelectron spectroscopy experiments, we reveal an entropy-driven phenomenon: the supported NPs redisperse into untrapped ADCs upon heating and reversibly sinter upon cooling in three systems (Pd-CeO2, Cu-TiO2, Ag-TiO2), contrary to the traditional understanding that \u201chigh temperature promotes sintering\u201d. We further establish the entropy-driven catalyst redispersion theory, analogous to two-dimensional dissolution, where thermodynamically stable ADCs are ubiquitous up to their saturation concentration. It redefines the basic understanding of sintering, dispersion, and coexistence behavior between NPs and ADCs, thereby offering multiple strategies for obtaining thermodynamically stable ADCs.<\/jats:p>","DOI":"10.1021\/jacs.6c04747","type":"journal-article","created":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T13:02:11Z","timestamp":1787144531000},"page":"36475-36484","source":"Crossref","is-referenced-by-count":0,"title":["Redefining Atomically\nDispersed Catalyst Stability\nvia Entropy"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0126-0854","authenticated-orcid":true,"given":"Beien","family":"Zhu","sequence":"first","affiliation":[{"name":"Shanghai Advanced Research Institute, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201210"]},{"name":"Shanghai Institute of Applied Physics, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201800"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiyuan","family":"Chen","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310027"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2934-1760","authenticated-orcid":true,"given":"Ying","family":"Jiang","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310027"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1719-4345","authenticated-orcid":true,"given":"Hui","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shanghai Advanced Research Institute, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201210"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Qi","sequence":"additional","affiliation":[{"name":"Shanghai Advanced Research Institute, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201210"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1297-784X","authenticated-orcid":true,"given":"Hongbo","family":"Zhao","sequence":"additional","affiliation":[{"name":"Shanghai Institute of Applied Physics, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201800"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaozhi","family":"Su","sequence":"additional","affiliation":[{"name":"Shanghai Advanced Research Institute, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201210"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8973-6561","authenticated-orcid":true,"given":"Zhi","family":"Liu","sequence":"additional","affiliation":[{"name":"ShanghaiTech University , , ,","place":["Shanghai, China, 201210"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3515-0642","authenticated-orcid":true,"given":"Bing","family":"Yang","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , 457 Zhongshan Road , , ,","place":["Dalian, Liaoning, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hiroaki","family":"Matsumoto","sequence":"additional","affiliation":[{"name":"Hitachi High-Tech (Shanghai) Co., Ltd. , ,","place":["Shanghai, P. R. China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chaobin","family":"Zeng","sequence":"additional","affiliation":[{"name":"Hitachi High-Tech (Shanghai) Co., Ltd. , ,","place":["Shanghai, P. R. China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7450-789X","authenticated-orcid":true,"given":"Wentao","family":"Yuan","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310027"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5968-9223","authenticated-orcid":true,"given":"Hangsheng","family":"Yang","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310027"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ze","family":"Zhang","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310027"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9893-8296","authenticated-orcid":true,"given":"Yong","family":"Wang","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310027"]},{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]},{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6015-5694","authenticated-orcid":true,"given":"Yi","family":"Gao","sequence":"additional","affiliation":[{"name":"Shanghai Advanced Research Institute, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201210"]},{"name":"Shanghai Institute of Applied Physics, Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201800"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,19]]},"reference":[{"key":"2026090312101584800_cit1","doi-asserted-by":"publisher","first-page":"1720","DOI":"10.1021\/ar3002427","article-title":"Sintering of Catalytic\nNanoparticles: Particle Migration or Ostwald Ripening?","volume":"46","author":"Hansen","year":"2013","journal-title":"Acc. 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Catal."},{"key":"2026090312101584800_cit18","doi-asserted-by":"publisher","first-page":"638","DOI":"10.1093\/nsr\/nwy094","article-title":"Theoretical\nUnderstanding of the Stability of Single-Atom Catalysts","volume":"5","author":"Liu","year":"2018","journal-title":"Nat. Sci. Rev."},{"key":"2026090312101584800_cit19","doi-asserted-by":"publisher","first-page":"150","DOI":"10.1126\/science.aaf8800","article-title":"Thermally Stable Single-Atom Platinum-on-Ceria Catalysts via Atom\nTrapping","volume":"353","author":"Jones","year":"2016","journal-title":"Science"},{"key":"2026090312101584800_cit20","doi-asserted-by":"publisher","first-page":"856","DOI":"10.1038\/s41565-018-0197-9","article-title":"Direct Observation of\nNoble Metal Nanoparticles Transforming to Thermally\nStable Single Atoms","volume":"13","author":"Wei","year":"2018","journal-title":"Nat. Nanotechnol."},{"key":"2026090312101584800_cit21","doi-asserted-by":"publisher","first-page":"8460","DOI":"10.1021\/acscatal.7b03090","article-title":"Chemical Potential\nof Metal Atoms in Supported Nanoparticles: Dependence\nupon Particle Size and Support","volume":"7","author":"Campbell","year":"2017","journal-title":"ACS Catal."},{"key":"2026090312101584800_cit22","doi-asserted-by":"publisher","first-page":"851","DOI":"10.1038\/s41565-019-0518-7","article-title":"High Temperature Shockwave\nStabilized Single Atoms","volume":"14","author":"Yao","year":"2019","journal-title":"Nat. Nanotechnol."},{"key":"2026090312101584800_cit23","doi-asserted-by":"publisher","first-page":"17364","DOI":"10.1021\/jacs.0c04887","article-title":"High-Temperature Pulse\nMethod for Nanoparticle Redispersion","volume":"142","author":"Xie","year":"2020","journal-title":"J. Am.\nChem. Soc."},{"key":"2026090312101584800_cit24","doi-asserted-by":"publisher","first-page":"503","DOI":"10.1038\/s41929-022-00796-1","article-title":"Atomically Dispersed Pt and Fe Sites and Pt-Fe Nanoparticles for\nDurable Proton Exchange Membrane Fuel Cells","volume":"5","author":"Xiao","year":"2022","journal-title":"Nat. Catal."},{"issue":"1","key":"2026090312101584800_cit25","doi-asserted-by":"publisher","first-page":"981","DOI":"10.1038\/s41467-025-56339-2","article-title":"Silver Single Atoms and Nanoparticles\non Floatable Monolithic Photocatalysts for Synergistic Solar Water\nDisinfection","volume":"16","author":"Wang","year":"2025","journal-title":"Nat. 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C"},{"key":"2026090312101584800_cit32","doi-asserted-by":"publisher","first-page":"5502","DOI":"10.1021\/acscatal.2c06321","article-title":"Active Site\nEntropy of Atomically Dispersed Rh\/Al2O3 Catalysts\nDictates Activity for Ethylene Hydroformylation","volume":"13","author":"Zakem","year":"2023","journal-title":"ACS Catal."},{"key":"2026090312101584800_cit33","doi-asserted-by":"publisher","first-page":"21","DOI":"10.1016\/0079-6786(75)90013-8","article-title":"Supported Metal Crystallites","volume":"9","author":"Wynblatt","year":"1975","journal-title":"Prog. 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