Machine Learning Guided Assembly of a Nested Gd@Gd @Ni Cluster via Urea Controlled Carbonate Release.

Lanthanide-based polyhedral clusters are of great interest due to their unique geometries and functional properties, but their controlled synthesis remains a major challenge. Here, we report a nested three-shell cluster, [GdNi(MeIDA)(OH)(CO) (HO)]·(ClO)·(HO) (GdNi, HMeIDA = N-Methyliminodiacetic acid), achieved by using urea as a slow-release carbonate source to direct the formation of a dodecahedral inner shell. Single-crystal X-ray diffraction reveals a unique Gd@Gd@Ni arrangement, with the innermost Gd forming a Platonic dodecahedron templated by carbonate.