Evolution from Octahedral to Icosahedral Metal‐Organic Polyhedra Assembled by Two Types of Polyoxovanadate Clusters

Design and synthesis of metal‐organic polyhedra (MOPs) with targeted geometries from predetermined secondary building units (SBUs) is a long‐standing challenge in chemistry and material science. The theoretical prediction shows that there are 6 possible polyhedra from (3,4)–c octahedron to (3,5)–c icosahedron with minimal transitivity (simplest possible). Except missing one polyhedron (mtr) due to the unfavorable angles, we report five MOPs based on these structures, including an octahedral (3,4)‐c VMOP‐21 (rdo), an icosahedral (3,5)‐c VMOP‐25 (trc), and three intermediate derived trinodal (3,4,5)–c VMOP‐22~24 (ghm, hmg, xum). Remarkably, all these MOPs obey the minimal transitivitity principle and are well consistent with geometrical predictions.

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