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Metal-metal contacts in late transition metal polymers

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JYU dissertations
Authors
Kolari, Kalle
Date
2020

 
This thesis titled ‘Metal-metal contacts in late transition metal polymers’ contains two main parts: the introductory section, and a section presenting and discussing the key results of the study. A concluding section, summarising the study’s findings, is also provided. The introduction gives a classification of metallopolymers based on parameters such as structure, metal-ion bonding interaction with the polymeric framework, and electronic interactions that polymers may express. Additionally, structural and crystal-packing features of metallopolymers— namely, extended metal atom chains (EMACs)—are presented. Moreover, first section of the thesis contains a brief introduction to metal-metal interactions. It also describes the solid state structure of compounds in which group 11 (Cu, Ag and Au), Rh, and Pt contacts with aromatic N, S-, or N-donor ligands are present. Finally, properties and applications of metal-metal contact containing compounds are presented. The second main part of thesis presents the results of the syntheses and characterisation of group 11, Rh, and Pt polymers. Either ditopic bridging ligands or chelating polypyridines were utilised to promote polymeric structures with close metal-metal contacts. Nine compouds were synthesized and characterized with single crystal x-ray diffraction. Metal-metal contacts were analysed with computational chemistry, distance criteria, or spectroscopy. Metal-metal distances with a sub sum of Bondi’s Van der Waals radii were present in 8 of obtained structures. In addition to Pt-Pt contacts, platinum polymer were found to be luminescent and act as a metallogelator. Fluorophilic interactions were found to impact on gelation behaviour of metallogelator. Mechanical and thermal stability and self-healing properties of obtained gel were investigated with rheology. In sum, the results presented highlight the great importance of ligand selection for the formation of structural and chemical features of one-dimensional polymeric materials that contain close metal-metal separations and interactions. ...
 
Väitöskirja Metalli-metalli kontaktit siirtymämetalli polymeereissä jakautuu kahteen osaan: Johdantoon sekä tuloksiin ja johtopäätöksiin. Johdanto-osiossa käydään läpi väitöskirjatyön kannalta keskeisimpiä aihealueita, joihin kuuluvat metallopolymeerit sekä metalli-metalli vuorovaikutukset. Metallopolymeerit kappaleessa havainnollistetaan yhdisteryhmille keskeisimmät luokittelutavat sekä rakenteelliset ominaisuudet. Metalli-metalli vuorovaikutusten muodostumismekanismia käsitellään lyhyesti yhdisteille tyypillisimpien ominaisuuksien sekä sovelluskohteiden ohessa. Tulokset ja johtopäätökset kappale sisältää väitöskirjatyön keskeisimmät tulokset. Ryhmän 11, Rh sekä Pt metallopolymeerejä syntetisoitiin käyttäen joko ditooppista metalleja silloittavaa pyridiini-4-tiolia tai kelatoivia polypyridiini ligandeja. Yhdeksän yhdistettä syntetisoitiin sekä karakterisoitiin muun muassa röntgenkristallografian avulla. Metalli-metallikontakteja analysoitiin laskennallisella kemialla, etäisyyskriteerillä tai spektroskooppisesti. Kahdeksalla yhdisteistä, metalli-metalli kontaktien havaittiin olevan lyhyempiä kuin Bondin Van der Waals säteiden summat. Platina polymeeri havaittiin olevan myös luminesoiva sekä metallogelaattori. Fluorofiiliset vuorovaikutukset havaittiin vaikuttavan metallogelaattorin geelinmuodostamiskykyyn. Geelin mekaaniset, termiset sekä itsestään korjautuvuus ominaisuudet tutkittiin reologia menetelmällä. Tulokset korostavat ligandin valitsemisen tärkeyttä rakenteen sekä kemiallisten ominaisuuksien räätälöinnin näkökulmasta metalli-metallikontakteja sisältävissä yhdisteissä. ...
 
ISBN
978-951-39-8162-4
Contains publications
  • Artikkeli I: Kolari, K., Sahamies, J., Kalenius, E., Novikov, A. S., Kukushkin, V. Y., & Haukka, M. (2016). Metallophilic interactions in polymeric group 11 thiols. Solid State Sciences, 60 (October), 92-98. DOI: 10.1016/j.solidstatesciences.2016.08.005. JYX: jyx.jyu.fi/handle/123456789/51124.
  • Artikkeli II: Kolari, Kalle; Laurila, Elina; Chernysheva, Maria; Hirva, Pipsa; Haukka, Matti (2020). Self-assembly of square planar rhodium carbonyl complexes with 4,4-disubstituted-2,2’-bipyridine ligands. Solid State Sciences, 100, 106103. DOI: 10.1016/j.solidstatesciences.2019.106103. JYX: jyx.jyu.fi/handle/123456789/67415.
  • Artikkeli III: Kolari, Kalle; Bulatov, Evgeny; Tatikonda, Rajendhraprasad; Bertula, Kia; Kalenius, Elina; Nonappa; Haukka, Matti (2020). Self-healing, luminescent metallogelation driven by synergistic metallophilic and fluorine–fluorine interactions. Soft matter, 16 (11), 2795-2802. DOI: 10.1039/C9SM02186H
Keywords
polymeerit metallit geelit kompleksiyhdisteet kemialliset sidokset kemiallinen synteesi optiset ominaisuudet fysikaaliset ominaisuudet metallopolymers metal-metal contacts metal-metal interactions
URI

http://urn.fi/URN:ISBN:978-951-39-8162-4

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