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Passive thermal energy storage systems using microencapsulated phase change materials (PCMs) offer promise but face integration challenges in cementitious materials due to weakening mechanical strength, which arises from poor shell strength and weak interfacial bonding with cementitious phases. This study introduces a novel approach for synthesizing functionalized microencapsulated PCMs from fly ash\u2010based cenospheres addressing interfacial compatibility. Cenospheres are perforated for PCM encapsulation and sealed using two different materials: 1) melamine\u2010formaldehyde (MF), a standard polymeric shell; and 2) silica, selected for its chemical compatibility with cementitious phases. Experimental results show that the silica sealing improved mechanical strength by 50% over those of MF, corroborated by molecular dynamic simulations showing silica's binding energy with calcium silicate hydrate exceeded threefold, with more than twice the uniaxial tensile strength. Thermal analyses confirmed the preservation of PCM in both sealing approaches. This work establishes a transformative pathway for advancing PCM\u2010based thermal energy storage in building materials.<\/jats:p>","DOI":"10.1002\/advs.202417350","type":"journal-article","created":{"date-parts":[[2025,4,11]],"date-time":"2025-04-11T09:36:37Z","timestamp":1744364197000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Surface\u2010Engineered Cenospheres Encapsulating Phase Change Materials for Functional Cementitious Composites"],"prefix":"10.1002","volume":"12","author":[{"given":"Sahand","family":"Rahemipoor","sequence":"first","affiliation":[{"name":"Department of Civil and Mechanical Engineering Technical University of Denmark  Kgs Lyngby 2800 Denmark"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Carsten","family":"Kuenzel","sequence":"additional","affiliation":[{"name":"Department of Civil and Environmental Engineering Imperial College London  London SW72AZUK UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Toms","family":"Valdem\u0101rs Eiduks","sequence":"additional","affiliation":[{"name":"Institute of Physics and Materials Science Faculty of Natural Sciences And Technology at Riga Technical University  3 P. Valdena Str. Riga LV\u20101048 Latvia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Andrei","family":"Shishkin","sequence":"additional","affiliation":[{"name":"Institute of Physics and Materials Science Faculty of Natural Sciences And Technology at Riga Technical University  3 P. Valdena Str. Riga LV\u20101048 Latvia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mohammadreza","family":"Izadifar","sequence":"additional","affiliation":[{"name":"Institute of Construction and Building Materials Technical University of Darmstadt  64287 Darmstadt Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Neven","family":"Ukrainczyk","sequence":"additional","affiliation":[{"name":"Institute of Construction and Building Materials Technical University of Darmstadt  64287 Darmstadt Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Eduardus","family":"Koenders","sequence":"additional","affiliation":[{"name":"Institute of Construction and Building Materials Technical University of Darmstadt  64287 Darmstadt Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1485-3931","authenticated-orcid":false,"given":"Navid","family":"Ranjbar","sequence":"additional","affiliation":[{"name":"Department of Civil and Mechanical Engineering Technical University of Denmark  Kgs Lyngby 2800 Denmark"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,4,11]]},"reference":[{"key":"e_1_2_8_1_1","unstructured":"Eurostat Energy Consumption in Households2024."},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.rser.2016.03.036"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.rser.2021.110751"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202309850"},{"key":"e_1_2_8_5_1","volume":"34","author":"Lee J.","year":"2024","journal-title":"Adv. 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