Dental　amalgam,　known　for　its　biocompatibility　and　ductility,　is　widely　used　in　restorative　materials.　In　dental　crown　restorations,　studying　the　interactions　between　amalgam　fillings　and　crown　tissues,　particularly　the　roles　of　calcium　(Ca)　and　strontium　(Sr),　is　essential　for　improving　function　stability　and　biocompatibility.　This　study　conducts　critical　literature　evaluation　and　thermodynamic　optimization　of　binary　systems　involving　mercury　(Hg)　with　Ca　and　Sr,　focusing　specifically　on　their　suitability　for　dental　amalgam　restoration.　Using　first-principles　calculations　(FPC),　the　enthalpies　of　formation　for　compounds　within　the　Hg-Ca　and　Hg-Sr　binary　systems　were　calculated　in　this　work.　Thermodynamic　modeling　of　the　liquid　solution　employed　the　modified　quasichemical　model　in　the　pair　approximation　(MQM),　uncovering　significant　short-range　ordering.　Conversely,　solid　phases　were　modeled　using　the　compound　energy　formalism　(CEF).　The　incorporation　of　FPC　proves　to　be　a　valuable　and　effective　method,　providing　essential　insights　to　complement　the　calculation　of　phase　diagrams　(CALPHAD)　modeling　approach.　Ultimately,　this　research　significantly　enhances　our　understanding　of　the　thermodynamic　characteristics　of　Hg-X　alloys,　with　notable　implications　for　their　potential　application　in　dental　amalgam　restoration.　©　2024　Elsevier　Ltd