Catalytic Dehydrogenative Silylation of Alkenes by a well-defined MOF-Supported Silylphosphine Rh(III) Complex

29 April 2025, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

The transmetallation reaction of [ClRh(kappa3(P,Si,Si)-PhP(2-C6H4CH2SiiPr2)2)], Rh-1, with lithiated NU-1000 lead to grafting of the [Rh(kappa3(P,Si,Si)-PhP(2-C6H4CH2SiiPr2)2)] moiety within the porous structure of NU-1000 through Rh-O-Zr bonds and creating a robust heterogeneous catalyst for the dehydrogenative silylation of styrene and its derivatives. Compared to its homogeneous counterpart, Rh@NU-1000 exhibits enhanced selectivity, recyclability, and stability. The improved robustness is attributed to the synergistic cooperation of the Rh(III) center with the NU-1000 porous framework, enhancing substrate accessibility under milder conditions.

Keywords

dehydrogenative silylation
hydrosilation
Metal Organic Framework
grafted MOFs
rhodium
14-electron complex
silylphosphines

Supplementary materials

Title
Description
Actions
Title
Experimental NMR, IR, XAS
Description
Experimental section, materials and methods, NMR spectra of Rh-1 and metallation products and of catalytic products. XANES, EXAFS, ICP-MS, SEM-EDS, IR.
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