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New peptide-type tripodal ligands and their metal complexes : synthesis, thermodynamic and structural study, application in catalytic function

Abstract : One of the most important directions of modern bioinorganic research is the development of artificial enzymes. One pathway of enzyme modeling strategy is the study of amino acid sequences present in the active centers of metalloenzymes. Linear peptides, however, have their limitations in reconstituting the active centers of metalloenzymes, since they do not possess the well-defined three dimensional structure, therefore their structure is vulnerable towards amide nitrogen coordination/hydrolysis. Improvement of metal binding capabilities of linear peptides can be obtained by e.g. their functionalization with tripodal ligands. Tripodal compounds may provide a rigid, less flexible platform for the coordinating amino acid side chains, creating pre-organized metal binding sites. In my thesis, I present synthesis and characterization of histidine containing tripodal peptide ligands and their complex formation in presence of copper(II) and zinc(II). Solution equilibrium was studied with pH potentiometric measurements, and several spectroscopic methods were used for structural characterization (UV-Vis, CD, ESR, NMR and MS methods). Beside thermodynamic and structural characterization, enzyme mimicking catalytical properties of the complexes have also been investigated (catechol oxidation, superoxide dismutation). Our results demonstrated that tripodal peptide ligands are capable of enhancing the stability of metal-peptide complexes, and they may provide convenient structures to efficiently mimic the catalytic functions of enzymes. With thorough and systematical solution equilibrium and spectroscopic studies, we uncovered the driving forces of metal coordination, and established the impact of the tripodal structure in stability, structure and catalytic properties of the forming complexes. Our findings confirm the beneficial effect of tripodal scaffolds in peptide-type ligand-metal complexes, and emphasize the possibilities lying within tripodal peptides in the field of enzyme mimicking
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Ágnes Dancs. New peptide-type tripodal ligands and their metal complexes : synthesis, thermodynamic and structural study, application in catalytic function. Coordination chemistry. Université de Lorraine; Szegedi Tudományegyetem, 2017. English. ⟨NNT : 2017LORR0292⟩. ⟨tel-01823686⟩

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