期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 23, 期 59, 页码 14769-14777出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201702113
关键词
homogeneous catalysis; hydroformylation; porphyrinoids; rhodium; supramolecular chemistry
资金
- Eastman Chemical Company
- European Research Council (ERC Adv. NAT-CAT Reek)
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.
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