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Unprecedented regioselectivity to the branched aldehyde product in the hydroformylation of propene was attained on embedding a rhodium complex in supramolecular assembly  L2 , formed by coordination‐driven self‐assembly of tris( meta ‐pyridyl)phosphine and zinc(II) porpholactone. The design of cage  L2  is based on the ligand‐template approach, in which the ligand acts as a template for cage formation. Previously, first‐generation cage  L1 , in which zinc(II) porphyrin units were utilized instead of porpholactones, was reported. Binding studies demonstrate that the association constant for the formation of second‐generation cage  L2  is nearly an order of magnitude higher than that of  L1 . This strengthened binding allows cage  L2  to remain intact in polar and industrially relevant solvents. As a consequence, the unprecedented regioselectivity for branched aldehyde products can be maintained in polar and coordinating solvents by using the second‐generation assembly.

Tuning the Porphyrin Building Block in Self‐Assembled Cages for Branched‐Selective Hydroformylation of Propene