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Article Abstract
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. A machine learning-guided, high-throughput synthesis platform enabled the exploration of 780 reaction conditions, uncovering key parameters and phase boundaries governing cluster formation. This work demonstrates data-driven strategies can accelerate the discovery of complex lanthanide architectures.
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