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The ability to construct complex molecular architectures with precise control is critical for realizing molecule‐based materials and functions. Using the assembly of a 60‐metal complex of ErIII with histidine as an example, we demonstrate the rational assembly of otherwise synthetically elusive polynuclear lanthanide hydroxide clusters directed by the combined set of I− and CO32− as templates. We succeeded in the stepwise transformation starting from Er12 to Er60 by way of two key intermediates Er34 and Er48. The Er12, Er34, and Er48 core motifs represent respectively 1/6, 1/2, and 3/4 of the complete sodalite cage of Er60. This work, representing a rare example of rationally constructing high‐nuclearity lanthanide clusters guided by judiciously chosen templates, is expected to stimulate more future efforts for the controllable synthesis of complex molecular or supramolecular architectures with unprecedented structural sophistication and possibly useful properties. [ABSTRACT FROM AUTHOR]

Anion Template, Clusters, Lanthanides, Polynuclear, Self-Assembly In their Research Article (e202205385), Min Feng, Zhiping Zheng, and co-workers developed a stepwise synthesis of a high-nuclearity sodalite cage-like cluster B Er b SB B 60 b sb , guided by judiciously selected anions. Keywords: Anion Template; Clusters; Lanthanides; Polynuclear; Self-Assembly EN Anion Template Clusters Lanthanides Polynuclear Self-Assembly 1 1 1 08/11/22 20220815 NES 220815 B The rational synthesis b of high-nuclearity lanthanide clusters remains challenging. [Extracted from the article]

The ability to construct complex molecular architectures with precise control is critical for realizing molecule‐based materials and functions. Using the assembly of a 60‐metal complex of ErIII with histidine as an example, we demonstrate the rational assembly of otherwise synthetically elusive polynuclear lanthanide hydroxide clusters directed by the combined set of I− and CO32− as templates. We succeeded in the stepwise transformation starting from Er12 to Er60 by way of two key intermediates Er34 and Er48. The Er12, Er34, and Er48 core motifs represent respectively 1/6, 1/2, and 3/4 of the complete sodalite cage of Er60. This work, representing a rare example of rationally constructing high‐nuclearity lanthanide clusters guided by judiciously chosen templates, is expected to stimulate more future efforts for the controllable synthesis of complex molecular or supramolecular architectures with unprecedented structural sophistication and possibly useful properties. [ABSTRACT FROM AUTHOR]