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To unlock their full potential a primary challenge is the development of redox stable, coking tolerant and catalytically active mixed ionic and electronic conducting (MIEC) materials. Here, we have functionalized a robust lanthanum strontium iron chromate by introducing both A-site deficiency to increase the number of oxygen vacancies and surface exchange kinetics, as well as Ni-doping at the B-site to boost catalytic properties by exsolving FeNi-based alloy nanoparticles. The morphological analysis revealed the high thermal stability of the host perovskite and the successful decoration of its surface with an Fe-rich, FeNi alloy as identified by the HRTEM analysis after reduction at 900 \u00b0C for 12 h. The physicochemical characterizations revealed a significant enhancement of the electrocatalytic properties of the modified samples that resulted in an &amp;gt;40% decrease in electrode polarization resistance in CO2\/H2O co-electrolysis conditions. Our approach shows that simple yet rational modifications of highly stable perovskite oxides in combination with nano-engineering through exsolution could have a significant effect for advancing MIEC electrodes in SOECs.<\/jats:p>","DOI":"10.1021\/acsami.6c17672","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T10:01:29Z","timestamp":1792058489000},"page":"57708-57719","source":"Crossref","is-referenced-by-count":0,"title":["Functionalizing Robust (La,Sr)(Cr,Fe,Ni)O3 Mixed Ionic-Electronic Conducting Electrocatalysts through Bimetallic FeNi-Based Exsolution for Solid Oxide Electrolysis"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0831-0383","authenticated-orcid":true,"given":"Athanasios","family":"Zarkadoulas","sequence":"first","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alessia","family":"De Gregorio","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-1374-3602","authenticated-orcid":true,"given":"Eirini","family":"Marousiadou","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nannan","family":"Li","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Konstantinos","family":"Kotoulas","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Jiang","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8232-2083","authenticated-orcid":true,"given":"Francesco","family":"Picchioni","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7088-1160","authenticated-orcid":true,"given":"Vasileios","family":"Kyriakou","sequence":"additional","affiliation":[{"name":"University of Groningen , , Nijenborgh 3 , ,","place":["Groningen, The Netherlands, 9747 AG"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,15]]},"reference":[{"issue":"1","key":"2026102802074380800_cit1","doi-asserted-by":"publisher","DOI":"10.1115\/1.3005549","article-title":"Syngas Production via High-Temperature Coelectrolysis of Steam and Carbon Dioxide","volume":"6","author":"Stoots","year":"2009","journal-title":"J. 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