Palladium and copper complexes based on dendrimeric and monofunctional N, N’ chelating ligands as potential catalysts in the oxidative carbonylation of alcohols

Mketo, Nomvano (2010-03)

Thesis (MSc (Chemistry and Polymer Science))--University of Stellenbosch, 2010.

Thesis

ENGLISH ABSTRACT: In this thesis we describe the synthesis of several new N-(n-propyl)-1-(2-pyridyl and quinolyl)-imine ligands (ML1-ML4) as well as peripheral functionalised iminopyridyl and iminoquinolyl poly(propylene-imine) dendrimeric ligands (DL1-DL8) with a 1,4- diaminobutane core. The dendrimeric ligands were obtained by modification of the peripheral groups of Generation 1 and Generation 2 poly(propylene-imine) dendrimers, (DAB-(NH2)n which are commercially available, with a series of aldehydes. All the ligands were fully characterised by ESI-mass spectrometry, elemental analysis, 1H&13C{1H}-NMR, FT-IR and UV/Vis spectroscopies. These ligands were utilised to synthesise Pd(II) and Cu(I) complexes using appropriate metal precursors. Some of mononuclear complexes, [N-(n-propyl)-(2-pyridyl and quinolyl) methanimine] dichloro Pd(II) complexes (C1-C4) and bis[N-(n-propyl)-(2-pyridyl and quinolyl) methanimine] copper(I) tetrafluoroborate complexes (C14) were structurally characterised. Pd(II) complexes adopted a distorted square-planar geometry around the metal centre while Cu(I) complex exhibit a distorted tetrahedral arrangement around the metal centre. Both Pd(II) and Cu(I) multinuclear complexes (metallodendrimers) were characterised using a range of analytical techniques.

AFRIKAANSE OPSOMMING: In hierdie tesis word die sintese van verskeie nuwe N-(n-propiel)-1-(2-piridiel) en kinolielimien ligande (ML1-ML4) sowel as gefunksioneerde imienopiridiel en imienokinoliel poli(propilien-imien) dendrimeriese ligande (DL1-DL8) beskryf. Die dendrimeriese ligande was behaal deur die modifikasie van perifere groepe van Generasie 1 en Generasie 2 poli(propilien-imien) dendrimere met ‘n reeks aldehiede. Alle ligande was volledig deur ESI-massaspektrometrie, elementele analiese, 1H en 13C{1H} – KMR, FT-IR en UV/Sigbare spektroskopie gekarakteriseerd. Hierdie ligande was gebruik om Pd(II) en Cu(I) komplekse te berei om van die gepaste metaal voorlopers te gebruik te maak. Sommige van die mono-kern komplekse, [N-(npropiel)-( 2-piridiel) en kinoliel metanimien] dikloor Pd(II), komplekse (C1-C4) en bis[N-(npropiel)-( 2-piridiel) metanimien] koper(I) tetrafloorboraat, kompleks (C14) was struktureël gekarakteriseerd. Pd(II) komplekse neem ‘n versteurde vierkant valk geometrie om die metaal senter aan, terwyl die Cu(I) kompleks, ‘n versteurde tetrahedriese opset rondom die metaal toon. Beide Pd(II) en Cu(I) multikern komplekse (metaaldendrimere) was deur ‘n verskeidenheid van analitiese tegnieke gekarakteriseerd.

Please refer to this item in SUNScholar by using the following persistent URL: http://hdl.handle.net/10019.1/4288
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