Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium Complexes

The synthesis and characterization of the tripodal phosphines RSi(CH<sub>2</sub>CH<sub>2</sub>PPh<sub>2</sub>)<sub>3</sub> (R = Me, OMe, OEt) (<b>1</b>–<b>3</b>) is described. The <sup>1</sup>H NMR spectra of all pho...

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Main Authors: Maxwell R. Kimball, Kyle J. Cluff, Nattamai Bhuvanesh, Janet Blümel
Format: Article
Language:English
Published: MDPI AG 2025-04-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/30/7/1616
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author Maxwell R. Kimball
Kyle J. Cluff
Nattamai Bhuvanesh
Janet Blümel
author_facet Maxwell R. Kimball
Kyle J. Cluff
Nattamai Bhuvanesh
Janet Blümel
author_sort Maxwell R. Kimball
collection DOAJ
description The synthesis and characterization of the tripodal phosphines RSi(CH<sub>2</sub>CH<sub>2</sub>PPh<sub>2</sub>)<sub>3</sub> (R = Me, OMe, OEt) (<b>1</b>–<b>3</b>) is described. The <sup>1</sup>H NMR spectra of all phosphines display virtual coupling patterns. The ligands form the corresponding trinuclear Pd complexes [RSi(CH<sub>2</sub>CH<sub>2</sub>PPh<sub>2</sub>)<sub>3</sub>]<sub>2</sub>(PdCl<sub>2</sub>)<sub>3</sub> (<b>4</b>–<b>6</b>) with three PdCl<sub>2</sub> moieties sandwiched between two tripodal ligands. The complexes <b>4</b>, <b>5</b>, and <b>7</b> (R = OH) have been analyzed by single crystal X-ray diffraction. The coordination at the Pd center is square planar with the phosphine groups occupying <i>trans</i> positions. The <sup>31</sup>P{<sup>1</sup>H} MAS NMR spectra of polycrystalline <b>1</b> are in accordance with the packing motif of the molecules in the unit cell. The tripodal ligand <b>3</b> has successfully been immobilized on silica as <b>3i</b>. It coordinates PdCl<sub>2</sub> on the surface, as demonstrated by <sup>31</sup>P{<sup>1</sup>H} MAS NMR. Hereby, the <i>cis</i> coordination is prevalent when <b>3i</b> has maximal surface coverage. At low surface coverage, one tripodal linker can accommodate <i>trans</i> coordination at the metal center. A surface-bound trinuclear Pd complex has been generated, as well as a heterobimetallic Pd/Cu complex. All surface species have been characterized by <sup>31</sup>P{<sup>1</sup>H} MAS NMR.
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spelling doaj-art-d296a776670e4116ae012031f8e86ee72025-08-20T02:09:19ZengMDPI AGMolecules1420-30492025-04-01307161610.3390/molecules30071616Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium ComplexesMaxwell R. Kimball0Kyle J. Cluff1Nattamai Bhuvanesh2Janet Blümel3Department of Chemistry, Texas A&M University, College Station, TX 77842-3012, USADepartment of Chemistry, Texas A&M University, College Station, TX 77842-3012, USADepartment of Chemistry, Texas A&M University, College Station, TX 77842-3012, USADepartment of Chemistry, Texas A&M University, College Station, TX 77842-3012, USAThe synthesis and characterization of the tripodal phosphines RSi(CH<sub>2</sub>CH<sub>2</sub>PPh<sub>2</sub>)<sub>3</sub> (R = Me, OMe, OEt) (<b>1</b>–<b>3</b>) is described. The <sup>1</sup>H NMR spectra of all phosphines display virtual coupling patterns. The ligands form the corresponding trinuclear Pd complexes [RSi(CH<sub>2</sub>CH<sub>2</sub>PPh<sub>2</sub>)<sub>3</sub>]<sub>2</sub>(PdCl<sub>2</sub>)<sub>3</sub> (<b>4</b>–<b>6</b>) with three PdCl<sub>2</sub> moieties sandwiched between two tripodal ligands. The complexes <b>4</b>, <b>5</b>, and <b>7</b> (R = OH) have been analyzed by single crystal X-ray diffraction. The coordination at the Pd center is square planar with the phosphine groups occupying <i>trans</i> positions. The <sup>31</sup>P{<sup>1</sup>H} MAS NMR spectra of polycrystalline <b>1</b> are in accordance with the packing motif of the molecules in the unit cell. The tripodal ligand <b>3</b> has successfully been immobilized on silica as <b>3i</b>. It coordinates PdCl<sub>2</sub> on the surface, as demonstrated by <sup>31</sup>P{<sup>1</sup>H} MAS NMR. Hereby, the <i>cis</i> coordination is prevalent when <b>3i</b> has maximal surface coverage. At low surface coverage, one tripodal linker can accommodate <i>trans</i> coordination at the metal center. A surface-bound trinuclear Pd complex has been generated, as well as a heterobimetallic Pd/Cu complex. All surface species have been characterized by <sup>31</sup>P{<sup>1</sup>H} MAS NMR.https://www.mdpi.com/1420-3049/30/7/1616tripodal phosphinesimmobilized phosphinestrinuclear Pd complexesvirtual couplingsimmobilized Pd complexes<i>cis</i>- and <i>trans</i>-coordinated Pd complexes
spellingShingle Maxwell R. Kimball
Kyle J. Cluff
Nattamai Bhuvanesh
Janet Blümel
Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium Complexes
Molecules
tripodal phosphines
immobilized phosphines
trinuclear Pd complexes
virtual couplings
immobilized Pd complexes
<i>cis</i>- and <i>trans</i>-coordinated Pd complexes
title Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium Complexes
title_full Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium Complexes
title_fullStr Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium Complexes
title_full_unstemmed Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium Complexes
title_short Molecular and Immobilized Tripodal Phosphine Ligands and Their Trinuclear Palladium Complexes
title_sort molecular and immobilized tripodal phosphine ligands and their trinuclear palladium complexes
topic tripodal phosphines
immobilized phosphines
trinuclear Pd complexes
virtual couplings
immobilized Pd complexes
<i>cis</i>- and <i>trans</i>-coordinated Pd complexes
url https://www.mdpi.com/1420-3049/30/7/1616
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