Synthesis and efficacy of square planar copper complexes designed to nucleate Beta-sheet structure /

The synthesis of four 6,6'-bis(acylamino)-2,2'-bipyridine-

Bibliographic Details
Main Author: Schneider, Joel Patrick, 1968-
Format: Thesis Book
Language:English
Published: [Place of publication not identified] : [publisher not identified] ; 1995.
Subjects:
Online Access:Link to OAKTrust copy
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Description
Summary:The synthesis of four 6,6'-bis(acylamino)-2,2'-bipyridine-
based amino acids la-c and 2 are described. These residues,
when coordinated to Cu(II), are designed to replace the i + I
and i + 2 residues of a []-turn. Amino acids la-c and 2 were
incorporated into several different peptides to evaluate
their efficacy as 0-sheet nucleators. Matrix assisted laser
desorption mass spectroscopy and UV spectroscopy reveal that
peptides incorporating these residues bind CU(II) ions under
alkaline and acidic conditions with a 1: 1 binding
stoichiometry. In an effort to predict the geometry of the
metal binding site of peptides containing 0-turn mimics la-c
and 2, three model compounds, 19, 20, and 21 were prepared
and their crystal structures determined. The crystal
structure of 6,6'-bis(phenylacetamide)-2,2-bipyridine (19)
suggests that the bipyridine rings of peptides containing
these residues should exist in a transoid conformation in the
absence of CU(II) ions and other stabilizing forces. The
crystal structures of neutral (deprotonated) Cu(II)complex 20
and +2 charged (protonated) Cu(II)-complex 21 suggest that
peptides containing residues la-c and 2 bind CU(II) ions
under alkaline and acid conditions resulting in a cisoid
bipyridine ring conformation with a nearly perfect square
planar geometry about the copper atom. Spectroscopic studies
on peptides incorporating residue 1B indicate that this
residue is capable of nucleating an antiparallel 0-sheet
conformation upon binding a single CU(II) ion in basic
aqueous buffer. Peptides incorporating residue 2 behave
differently than those containing residue 1B in that they are
capable of adopting an antiparallel 0-sheet conformation
either in the absence or presence of CU(II) ions. The
chemical structure of residue 2 is such that the cisoid
nucleating conformation may be stabilized by hydrophobic
interactions in the absence of transition metal binding.
Item Description:Vita.
"Major Subject: Chemistry".
In title, symbol for Greek letter Beta is used.
Physical Description:xi, 102 leaves : illustrations ; 28 cm.
Issued also on microfiche from University Microfilms Inc.
Bibliography:Includes bibliographical references.