Date of Award

12-1976

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Legacy Department

Chemistry

First Advisor

John F Gelran

Second Advisor

H. Saith Spencer

Third Advisor

Farrell B. Brown

Abstract

The unsymmetrical, heterocyclic, secondary amines, 2-pyridyl-2'-pyrimidylamine (HPPA), 2-pyridyl-2'-thiazolylamine (HPTA), 2-pyridyl-2'-(4 -methylthiazolyl)amine (HMPTA), and 2-(6-methylpyridyl)-2 ' -(4-methylthiazolyl) amine (HDMPTA), have been prepared and characterized by analysis and mass spectroscopy. All four amines act as bidentates in forming coordination compounds having the general formula, Cu(HL)2(Cl04)2, where the HL represents the neutral amine. Spectral and magnetic evidence indicates a pseudotetrahedral ligand field geometry in the solid state for all four compounds except the unstable HDMPTA complex. Upon solution the HPPA and HPTA compounds add two solvent molecules to the Cu2+ coordination sphere probably in a trans fashion; the HMPTA and HDMPTA complexes react irreversibly by an electrontransfer process. Cu(HPTA)2(ClO4)2 and Cu(HMPTA)2(ClO4)2 have each been deprotonated to give neutral compounds with the general formula, CuL 2, where L is the ligand anion. The solvent independent spectra of each complex are characteristic of pseudotetrahedral ligand fields. Hg(HPPA)2(ClO4)2, Hg(PPA)2, Pd(HPPA)2(ClO4)2, Pd(HPTA)2(CLO4)2, Pd(HMPTA)2(ClO4)2*2H2O, Pd(MPTA)2*H2O, Pd(HDMPTA)2(ClO4)2, and Pd(DMPTA)2*H20 have also been prepared and characterized. All of these compounds are diamagnetic. Attempts to prepare the 2:1 (amine:metal), HPTA, HMPTA, and HDMPTA Hg 2+ comp l exes resulted in polymeric compounds whose analyses indicated a ligand to metal ratio of 1.

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