Publication: Síntesis de sistemas polimetálicos biofuncionales
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2019-12-12
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Universidad Complutense de Madrid
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Abstract
La presente tesis doctoral se basa en el desarrollo de metodologías que permitan preparar estructuras que combinen metales de transición y biomoléculas. El trabajo se divide en dos partes claramente diferenciadas. Síntesis de miméticos de [FeFe]-hidrogenasas. Las [FeFe]-hidrogenasas son metaloenzimas esenciales en el metabolismo de ciertos microorganismos para la producción de H2. Los miméticos de [FeFe]-hidrogenasas han sido ampliamente estudiados en los últimos años y se han diseñado buscando la similitud estructural de sus centros activos con los complejos de tipo [(μ-SR)2Fe2(CO)6] de las metaloenzimas naturales, en particular los que presentan puentes azaditiolato (ADT) entre los átomos de azufre...
The main objective of this PhD thesis is the development of methodologies for the synthesis of structures combining transtition metal complexes and biomolecules. The work has been divided into 2 clearly differenciated parts. 1. Synthesis of [FeFe]-hydrogenase mimics. The mimics of these type of metaloenzymes, a very important class of enzymes related to the production of H2 in the metabolism of certain microorganisms, have been widely studied in the recent years, specially the ones with an aminodithiolate functionality in their structure like the one shown in Figure 1, due to the structural similarity of their active site and complexes like [(μ-SR)2Fe2(CO)6]. the redox properties asociated with the ADT-[FeFe] nucleus, regardless of the complexity of the structure incorporated through the cycloaddition reaction...
The main objective of this PhD thesis is the development of methodologies for the synthesis of structures combining transtition metal complexes and biomolecules. The work has been divided into 2 clearly differenciated parts. 1. Synthesis of [FeFe]-hydrogenase mimics. The mimics of these type of metaloenzymes, a very important class of enzymes related to the production of H2 in the metabolism of certain microorganisms, have been widely studied in the recent years, specially the ones with an aminodithiolate functionality in their structure like the one shown in Figure 1, due to the structural similarity of their active site and complexes like [(μ-SR)2Fe2(CO)6]. the redox properties asociated with the ADT-[FeFe] nucleus, regardless of the complexity of the structure incorporated through the cycloaddition reaction...
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Tesis inédita de la Universidad Complutense de Madrid, Facultad de Ciencias Químicas, Departamento de Química Orgánica I, leída el 12/11/2019