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Organic electrolytes offer a wider electrochemical stability window than aqueous ones but are typically limited to approximately 3 V. To enable high-voltage operation and long cycle life, the formation of stable passivation layers or interphases is essential. These interphases form through the precipitation of insoluble electrolyte decomposition products, driven by the collective behaviour of electrolyte components under battery conditions, where the cation solvation structure plays a crucial role in determining decomposition pathways. At the electrode\u2013electrolyte interface, steep potential gradients and altered solvation environments further influence interphase formation and decomposition mechanisms. This perspective examines the relationship between cation solvation structure and interphase composition, particularly for divalent cations (Ca\u00b2\u207a and Mg\u00b2\u207a), and highlights key areas for improvement in experimental protocols, electrolyte purity, and interphase characterization. Addressing these challenges will enhance both battery performance and the reliability and reproducibility of data in this emerging field.<\/jats:p>\n                  <jats:p>This article is part of the theme issue \u2018Electrolytes within the domain of electrochemistry and electrochemical energy storage\u2019.<\/jats:p>","DOI":"10.1098\/rsta.2025.0279","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T07:02:07Z","timestamp":1791442927000},"source":"Crossref","is-referenced-by-count":0,"title":["Ca and Mg batteries: tuning interphase and electrolyte stability through cation solvation structure"],"prefix":"10.1098","volume":"384","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0214-4115","authenticated-orcid":false,"given":"Deyana S.","family":"Tchitchekova","sequence":"first","affiliation":[{"name":"Institut de Ci\u00e8ncia de Materials de Barcelona (ICMAB-CSIC), Carrer dels Til.lers , 08193 Cerdanyola del Vall\u00e8s, Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7577-499X","authenticated-orcid":false,"given":"Tja\u0161a","family":"Pav\u010dnik","sequence":"additional","affiliation":[{"name":"Institut de Ci\u00e8ncia de Materials de Barcelona (ICMAB-CSIC), Carrer dels Til.lers , 08193 Cerdanyola del Vall\u00e8s, Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8232-6324","authenticated-orcid":false,"given":"Alexandre","family":"Ponrouch","sequence":"additional","affiliation":[{"name":"Institut de Ci\u00e8ncia de Materials de Barcelona (ICMAB-CSIC), Carrer dels Til.lers , 08193 Cerdanyola del Vall\u00e8s, Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"175","published-online":{"date-parts":[[2026,10,8]]},"reference":[{"key":"2026100803020355000_RSTA20250279C1","doi-asserted-by":"crossref","first-page":"966","DOI":"10.1063\/1.1742723","article-title":"On the theory of oxidation-reduction reactions involving electron transfer. 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