{"id":{"repo_id":"heid-diss","oai_identifier":"oai:archiv.ub.uni-heidelberg.de:6988"},"canonical_url":"https://search.dev.ndltd.org/etd/heid-diss/oai:archiv.ub.uni-heidelberg.de:6988","repository":{"repo_id":"heid-diss","name":"Universität Heidelberg","base_url":"http://archiv.ub.uni-heidelberg.de/volltextserver/cgi/oai2"},"display":{"title":"Toward Hydrogenase mimicry : subjecting the problem to three different approaches","abstract":"In this work, the challenging task of modelling Hydrogenase is subjected to three different approaches. The first strategy used here is bioorganometallic. A wide range of sulfur containing ferrocene-peptide derivatives were synthesized and fully characterized. As a second approach, organic self-assembled oligoquinoline were designed and synthesized. These two kind of structures were further used a scaffold for Hydrogenase mimics. In the third approach, a theoretical computational study of the ferrocene-peptide derivatives is led. In order to investigate a wider range of ferrocene-peptide as a molecular scaffold, a molecular force field was successfully implemented and validated for CHARMM. After the deprotection of the thiol group in the bioorganometallic approach, the free SH groups were coordinated with iron-carbonyl, so as to mimic the Fe-only Hydrogenase active site. The complexes thus obtained were comprehensively characterized and their electronic and electrochemical properties were extensively studied.","abstract_html":"In this work, the challenging task of modelling Hydrogenase is subjected to three different approaches. The first strategy used here is bioorganometallic. A wide range of sulfur containing ferrocene-peptide derivatives were synthesized and fully characterized. As a second approach, organic self-assembled oligoquinoline were designed and synthesized. These two kind of structures were further used a scaffold for Hydrogenase mimics. In the third approach, a theoretical computational study of the ferrocene-peptide derivatives is led. In order to investigate a wider range of ferrocene-peptide as a molecular scaffold, a molecular force field was successfully implemented and validated for CHARMM. After the deprotection of the thiol group in the bioorganometallic approach, the free SH groups were coordinated with iron-carbonyl, so as to mimic the Fe-only Hydrogenase active site. The complexes thus obtained were comprehensively characterized and their electronic and electrochemical properties were extensively studied.","abstract_has_math":false,"creators":["Hatten, Xavier Richard de"],"institution":"Universität Heidelberg","degree_name":null,"degree_level":"thesis.doctoral","degree_discipline":null,"degree_department":null,"school":null,"contributors":["Nils, Metzler-Nolte"],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2006,"date_issued":"2006-11-14","date_published":"2006-11-14","updated_at":"2026-07-24T02:30:34Z","subjects":[],"languages":[],"rights":[],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"http://www.ub.uni-heidelberg.de/archiv/6988","outbound_label":"Repository record","outbound_source":"source_url"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Nils, Metzler-Nolte"]},{"key":"dc:creator","label":"Author","values":["Hatten, Xavier Richard de"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:publisher","label":"Institution","values":["Universitätsbibliothek Heidelberg"]},{"key":"dc:type","label":"Dc Type","values":["doctoralThesis"]},{"key":"thesis:degree_level","label":"Degree Level","values":["thesis.doctoral"]},{"key":"thesis:institution_name","label":"Thesis Institution Name","values":["Universität Heidelberg"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description.abstract","label":"Abstract","values":["In this work, the challenging task of modelling Hydrogenase is subjected to three different approaches. The first strategy used here is bioorganometallic. A wide range of sulfur containing ferrocene-peptide derivatives were synthesized and fully characterized. As a second approach, organic self-assembled oligoquinoline were designed and synthesized. These two kind of structures were further used a scaffold for Hydrogenase mimics. In the third approach, a theoretical computational study of the ferrocene-peptide derivatives is led. In order to investigate a wider range of ferrocene-peptide as a molecular scaffold, a molecular force field was successfully implemented and validated for CHARMM. After the deprotection of the thiol group in the bioorganometallic approach, the free SH groups were coordinated with iron-carbonyl, so as to mimic the Fe-only Hydrogenase active site. The complexes thus obtained were comprehensively characterized and their electronic and electrochemical properties were extensively studied.","Le travail présenté dans cette thèse est dédié à la création de modèles du site actif des enzymes Hydrogénases. Cette problématique est soumise à trois approches différentes. La première stratégie utilisée est de type bioorganométallique. Un grand nombre de dérivés ferrocenoyl-peptide contenant des résidus soufrés (cystéine, méthionine) ont été synthétisés et caractérisés. Lors de la deuxième approche, concernant le domaine de la chimie organique, des hélices supramoléculaires à base d’oligoamides aromatiques ont été créées et isolées. Ces deux différents types de structures seront utilisés comme échelle moléculaire pour la création de modèle synthétique des enzymes Hydrogénases. La troisième approche consiste en l’étude théorique des composés ferrocenoyl-peptides, en utilisant la dynamique moléculaire. Un champ de force a été implémenté dans CHARMM concernant ces composés et validé avec succès. Les calculs de mécanique moléculaire sont utilisés pour étudier les différentes structures pouvant servir d’échelle moléculaire. Après déprotection des groupements thiols sur les dérivés obtenus lors de l’approche bioorganométallique, les groupements SH sont coordinnés à un centre ferrocarbonylé, reproduisant le site actif de l’enzyme « Fe-only Hydrogenase ». Les complexes ainsi obtenus ont été caractérisés et leur propriétés électroniques et électrochimiques largement étudiées."]},{"key":"dc:format.medium","label":"Dc Format Medium","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["Toward Hydrogenase mimicry : subjecting the problem to three different approaches","Drei neue Konzepte für strukturelle und funktionnelle Hydrogenase-Modelle"]}]}],"canonical_facts":{"dc:contributor":["Nils, Metzler-Nolte"],"dc:creator":["Hatten, Xavier Richard de"],"dc:description.abstract":["In this work, the challenging task of modelling Hydrogenase is subjected to three different approaches. The first strategy used here is bioorganometallic. A wide range of sulfur containing ferrocene-peptide derivatives were synthesized and fully characterized. As a second approach, organic self-assembled oligoquinoline were designed and synthesized. These two kind of structures were further used a scaffold for Hydrogenase mimics. In the third approach, a theoretical computational study of the ferrocene-peptide derivatives is led. In order to investigate a wider range of ferrocene-peptide as a molecular scaffold, a molecular force field was successfully implemented and validated for CHARMM. After the deprotection of the thiol group in the bioorganometallic approach, the free SH groups were coordinated with iron-carbonyl, so as to mimic the Fe-only Hydrogenase active site. The complexes thus obtained were comprehensively characterized and their electronic and electrochemical properties were extensively studied.","Le travail présenté dans cette thèse est dédié à la création de modèles du site actif des enzymes Hydrogénases. Cette problématique est soumise à trois approches différentes. La première stratégie utilisée est de type bioorganométallique. Un grand nombre de dérivés ferrocenoyl-peptide contenant des résidus soufrés (cystéine, méthionine) ont été synthétisés et caractérisés. Lors de la deuxième approche, concernant le domaine de la chimie organique, des hélices supramoléculaires à base d’oligoamides aromatiques ont été créées et isolées. Ces deux différents types de structures seront utilisés comme échelle moléculaire pour la création de modèle synthétique des enzymes Hydrogénases. La troisième approche consiste en l’étude théorique des composés ferrocenoyl-peptides, en utilisant la dynamique moléculaire. Un champ de force a été implémenté dans CHARMM concernant ces composés et validé avec succès. Les calculs de mécanique moléculaire sont utilisés pour étudier les différentes structures pouvant servir d’échelle moléculaire. Après déprotection des groupements thiols sur les dérivés obtenus lors de l’approche bioorganométallique, les groupements SH sont coordinnés à un centre ferrocarbonylé, reproduisant le site actif de l’enzyme « Fe-only Hydrogenase ». Les complexes ainsi obtenus ont été caractérisés et leur propriétés électroniques et électrochimiques largement étudiées."],"dc:format.medium":["application/pdf"],"dc:publisher":["Universitätsbibliothek Heidelberg"],"dc:title":["Toward Hydrogenase mimicry : subjecting the problem to three different approaches","Drei neue Konzepte für strukturelle und funktionnelle Hydrogenase-Modelle"],"dc:type":["doctoralThesis"],"thesis:degree_level":["thesis.doctoral"],"thesis:institution_name":["Universität Heidelberg"]},"updated_at":"2026-07-24T02:30:34Z"}