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

29 April 2025, Version 1
Working Paper
This content is an early or alternative research output and has not been peer-reviewed by Cambridge University Press at the time of posting.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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Version History

Apr 29, 2025 Version 1

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The content is available under CC BY NC ND 4.0 [opens in a new tab]

DOI

10.26434/chemrxiv-2025-v87rh
D O I: 10.26434/chemrxiv-2025-v87rh [opens in a new tab]

Funding

National Science Foundation
CHE-2102689
National Science Foundation
DBI-2215258
National Science Foundation
CHE-2310030
National Science Foundation
CHE/MCB 2304919
Department of Energy
DE-AC-02-06CH11357

Author’s competing interest statement

The author(s) have declared they have no conflict of interest with regard to this content

Ethics

The author(s) have declared ethics committee/IRB approval is not relevant to this content

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