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Дисертації з теми "Polypyridyl"

Автор: Grafiati

Опубліковано: 4 червня 2021

Оновлено: 21 лютого 2023

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1

Zheng, Sipeng. "The reactions of ruthenium (ii) polypyridyl complexes." Thesis, Nelson Mandela Metropolitan University, 2009. http://hdl.handle.net/10948/1089.

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Ruthenium (II) polypyridine complexes in general have been extensively studied because of their unique redox and photochemical properties. A typical example of such complexes is tris(2,2’-bipyridyl) ruthenium (II). In this study, this complex was synthesized and then characterized using electronic spectroscopy and cyclic voltammetry. It was also shown that the ruthenium concentration could be accurately determined using ICP-MS. It was found that the complex is very stable in various chemical environments. It was observed from spectrophotometric investigations that persulphate and lead dioxide easily oxidize Ru(bpy)3 2+ to Ru(bpy)3 3+ in the presence of heat and H2SO4, respectively. It was also observed that the oxidation between Ru(bpy)3 2+ and cerium (IV) occurred at approximately 3:2 [Ce(IV)]/[Ru(II)] mole ratio. The resultant Ru(bpy)3 3+ solution was unstable in the presence of light and recovery of Ru(bpy)3 2+ occurred gradually. The regeneration of Ru(bpy)3 2+ from Ru(bpy)3 3+ was found to be a multistep process, which appears to involve the formation of an intermediate species. The following reaction model was found to best explain the kinetic data obtained: Ru(bpy)3 2+ + Ce(IV) → Ru(bpy)3 3+ Ru(bpy)3 3+ → Ru(bpy)3 2+ Ru(bpy)3 3+ → Ru* intermediate Ru* intermediate → Ru(bpy)3 2+ Theoretical rate constants were also calculated for the same process under the experimental conditions. The comparison between the experimental and theoretical results gave good agreement. In addition, the factors that influence the rate of the regeneration of Ru(bpy)3 2+ from Ru(bpy)3 3+ were also discussed.

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2

Williams, R. Lee. "Ruthenium-Platinum Polypyridyl Complexes: Synthesis and Characterization." Thesis, Virginia Tech, 2001. http://hdl.handle.net/10919/44315.

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A series of bimetallic (RuII, PtII) complexes were synthesized with the general formula [(tpy)RuCl(BL)PtCl2](PF6) (tpy = 2,2':6',2"-terpyridine and BL = bridging ligand) and their spectroscopic, electrochemical, and DNA binding properties studied. The bridging ligands used in these complexes were 2,3-bis(2'-pyridyl)pyrazine (dpp), 2,3-bis(2'-pyridyl)quinoxaline (dpq) and 2,3-bis(2'-pyridyl)benzoquinoxaline (dpb). These complexes combine light-absorbing RuII-polypyridyl chromophores and a cis-PtCl2 structural motif known to bind DNA. The Ru-bound chloride may be substituted, enabling further modification of the spectroscopic properties. The synthesis of [(tpy)RuCl(BL)PtCl2](PF6) utilizes a building block approach that allows modifications to the series of complexes within the general synthetic scheme. This illustrates the applicability of this scheme to the development of new series of complexes. The lowest-energy absorption for the three complexes is assigned to a Ru(dp)-to-BL(p*) charge transfer transition. This transition shifts to lower energy as the ligand is varied from dpp to dpq to dpb. The first and second reductions are BL(0/-) and BL(-/2-) based and shift to more positive potentials from dpp to dpq to dpb. The Ru(II/III) redox couple remains at a nearly constant potential for the series. All three compounds show DNA binding when incubated with linearized plasmid DNA. Adduct formation was assessed by agarose gel electrophoresis as a retardation of band migration. when incubated with linearized plasmid DNA. Adduct formation was assessed by agarose gel electrophoresis as a retardation of band migration.
Master of Science

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3

Johansson, Olof. "Ruthenium(II) Polypyridyl Complexes : Applications in Artificial Photosynthesis." Doctoral thesis, Stockholm : Institutionen för organisk kemi, Univ, 2004. http://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-93.

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4

Jones, Lucy. "Two-photon applications of transition metal polypyridyl complexes." Thesis, University of Manchester, 2017. https://www.research.manchester.ac.uk/portal/en/theses/twophoton-applications-of-transition-metal-polypyridyl-complexes(a236f479-d27c-4a92-8b13-bfac51bb14d7).html.

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Materials that undergo two-photon absorbtion (2PA), the simultaneous absorption of two photons, are finding increasing use in many applications including 3D fluorescence microscopy, 3D data storage, and photodynamic therapy (PDT). For efficient use, a large two-photon cross-section is desired which can arise from centrosymmetric charge transfer in push-pull electron donor-acceptor (D-A) diads. These structural motifs have been applied to the construction of organic-based chromophores yielding materials with remarkably high two-photon absorption cross-sections, yet, few metal based examples have been studied. Hence, this thesis concerns research into enhanced two photon absorption and emission properties of d6 transition metal complexes bearing suitably structurally modified polypyridyl chromophores using a combination of experimental and theoretical data Two polar tolylterpyridyl-stilbene amine ligands, where NR2 = methyl and phenyl (1a and 1b respectively) have been synthesised and coordinated to a range of d6 transition metals as D-Ï-A-Ï-D motifs (RuII and IrIII) or D-Ï-A variations (ReI and PtII). A single crystal X-ray structure of ligand (1b) was obtained. Spectroscopic analysis indicated successful synthesis of all compounds. One photon luminescence spectroscopy indicated ligand centred emissions for all compounds. Unfortunately, 2PA measurements were unsuccessful for the compounds due to their weak emission and likely small cross-sections too low for the equipment available. Attempts at cis-trans isomerisation of the stilbene bond in the ligands 1a and 1b by UV irradiation were successful, and the isomerisation process was monitored by both UV-visible spectroscopy and 1H NMR spectroscopy. Two 5-substituted-1,10-phenanthroline ligands bearing fluorenyl units (7 and 8) were successfully coordinated to IrIII cyclometallated with phenylpyridine (ppy) and benzo-[H]-quinoline (pq). A single crystal X-ray structure was obtained for [Ir(ppy)2(7)][PF6] (7a). The complexes demonstrated strong emission originating from a triplet metal to ligand charge transfer (3MLCT) excited states due to their long lived luminescent lifetimes measured up to 2 Î1⁄4s. Quantum yields were measured up to 22 % and theie triplet oxygen quenching efficiencies were established by their Stern-Volmer quenching constants, KSV that were determined to be ca. 40 bar-1 and 60 bar-1 for the ppy complexes of 7 and 8 respectively. Preliminary in vitro experiments performed with C6 Glioma cells treated with [Ir(ppy)2(7)][PF6] (7a) show efficient sensitization for triplet oxygen (3O2) by two-photon excitation at 740 nm resulting in photodynamic effects which led to localised cell damage and death. This complex also demonstrated relatively high two-photon absorption cross-sections ranging from 50-80 Goeppert-Mayer units (GM) between 750 and 800 nm. Two new ReI complexes have been synthesised utilising the ligands 7 and 8 (7c and 8c). A single crystal X-ray structure was obtained for Re(CO)3(7)Cl. (7c) These complexes also exhibited relatively long luminescence lifetimes of ca. 300 ns originating from a 3MLCT state, but emission quantum yields were much lower than corresponding IrIII complexes. The Stern-Volmer quenching analysis demonstrated much less efficient quenching by 3O2, with KSV values of around 8 bar-1 for both compounds. A ligand containg a fluorenyl linker between two 5-substituted-1,10-phenanthroline units (9) has been utilised as a bridge for IrIII-ReI (9a) and IrIII- RuII (9b) complexes. Emission in these complexes arises from 3MLCT excited states and both exhibit dual component long lived luminescent lifetimes up to 1.3 Î1⁄4s and quantum yields around 22 %. KSV constants were measured at 23 and 41 bar-1 for Ir-Re (9a) and Ir-Ru (9b) respectively. Furthermore, the Ir-Ru complex demonstrated a markedly large two-photon cross-section of 350 GM at 730 nm.

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5

Smith, Nichola Ann. "Photoactivatable Ru(II) polypyridyl complexes as antibacterial agents." Thesis, University of Warwick, 2015. http://wrap.warwick.ac.uk/76173/.

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Novel photoactive ruthenium(II) complexes were designed to incorporate existing anti-tuberculosis drugs, isoniazid and nicotinamide, that could be released from the ruthenium(II) cage by photoactivation with visible light. Two sets of complexes were synthesised based on cis-[Ru(N-N')2(L)2][PF6]2and cis-[Ru(N-N')2(L)X][PF6], where N-N' is 2,2'-bipyridine (bpy) or 1,10-phenanthroline (phen), L is isoniazid (INH) or nicotinamide (NA) and X is either Cl or I. Their dynamic behaviour in solution was explored using NMR to probe the presence of atropisomers. In the case of cis-[Ru(bpy)2(NA)Cl][PF6] (1) and cis-[Ru(bpy)2(NA)I][PF6] (2), the rotation of NA is hindered on the NMR timescale at room temperature, behaviour that was surprisingly not observed for cis-[Ru(bpy)2(NA)2][PF6]2 (5). The hindered rotation was explored by computational methods (DFT) and revealed that hydrogen bonding between the halide and protons of the NA ligand hindered the rotation. The photochemical properties of the Ru(II) complexes were explored by UV-visible spectroscopy and liquid chromatography. All cis-[Ru(N-N')2(L)2][PF6]2complexes in aqueous solution release one ligand, L, in under 1 min using a blue LED (λirr = 463 nm, 50 mW cm- 2 ) to form the photoproduct cis-[Ru(N-N')2(L)(H2O)] 2+ . Continued photoirradiation releases a second ligand, L, with the production of various Ru(II) and Ru(III) aqua photoproducts (with both cis and trans geometry). Interestingly their production was dependent on the power of the light source. Complementary computational studies (DFT/TD-DFT) were utilised to understand structure-activity relationships with respect to photoactivity. The results from the calculations suggest that the number of key electronic transitions (notably1 MLCT) and the favourable leaving properties of the ligand, L, influence the rate of photorelease. In the latter case, a stronger p-accepting leaving ligand shifts the dissociative 3 MC state to lower energy, thus promoting more efficient ligand release. The photobiological properties of the Ru(II) complexes were explored by investigating binding to biomolecules and screening their antibacterial activity in vitro. The complex cis-[Ru(bpy)2(INH)2][PF6]2 (4) binds to the nucleobase 9-ethylguanine (9-EtG) after photoirradiation with a blue LED to produce cis-[Ru(bpy)2(INH)(9-EtG)] 2+ , however reaction with the amino acid L-cysteine was not observed. A 96-array blue LED (λirr = 465 nm, 20 mW cm-2 ) and 32-array multi-coloured LED (λirr = 465 nm, 520 nm, 589 nm and 625 nm, 5 mW cm-2 ) were designed in-house to screen the activity of the complexes in vitro. Their design and construction is described in detail. When tested against Mycobacterium smegmatis (a model for Mycobacterium tuberculosis), complexes cis-[Ru(bpy)2(INH)2][PF6]2 (4) and cis-[Ru(phen)2(INH)2][PF6]2 (6) showed the greatest activity upon photoirradiation for 1 min with a blue LED, with at least a 3x increase in potency when compared to the ligand alone, INH. Most importantly the complexes are inactive in the dark, showing that the antibacterial ligand is selectively released in vitro after photoirradiation. The complex cis-[Ru(bpy)2(MOPEP)2][PF6]2 (9), where MOPEP is 4-[2-(4-methoxyphenyl)ethynyl]pyridine, was initially designed to study two-photon activation via a femtosecond-pulsed laser. Surprisingly the complex was one-photon active with 600 nm and 800 nm light, due to the MOPEP ligand extending and increasing the intensity of the one-photon absorption band shoulder in the 600-800 nm region.

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6

Greguric, Antun, University of Western Sydney, of Science Technology and Environment College, and of Science Food and Horticulture School. "The DNA binding interactions of Ru(II) polypyridyl complexes." THESIS_CSTE_SFH_Greguric_A.xml, 2002. http://handle.uws.edu.au:8081/1959.7/620.

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This thesis reports on the synthesis, characterisation, enantiomeric resolution, 1H NMR structural study and physical evaluation of a series of certain bidentate ligand metal complexes, where ‘L-L’ denotes the ancillary bidentate ligand and ‘intercalator’ indicates the intercalating bidentate ligand. The L-L series varies in size and shape. Results of many tests and projects conducted are explained in detail.
Master of Science (Hons)

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7

McDonnell, Ursula J. "Synthesis and DNA Binding of Novel Ruthenium Polypyridyl Complexes." Thesis, University of Warwick, 2008. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.526217.

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8

Yang, Mei. "Iron(II) and ruthenium(II) polypyridyl complexes as photosensitizers." Available to US Hopkins community, 2003. http://wwwlib.umi.com/dissertations/dlnow/3080801.

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9

Greguric, Antun. "The DNA binding interactions of Ru(II) polypyridyl complexes." Thesis, View thesis View thesis, 2002. http://handle.uws.edu.au:8081/1959.7/620.

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This thesis reports on the synthesis, characterisation, enantiomeric resolution, 1H NMR structural study and physical evaluation of a series of certain bidentate ligand metal complexes, where ‘L-L’ denotes the ancillary bidentate ligand and ‘intercalator’ indicates the intercalating bidentate ligand. The L-L series varies in size and shape. Results of many tests and projects conducted are explained in detail.

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10

Greguric, Antun. "The DNA binding interactions of Ru(II) polypyridyl complexes /." View thesis View thesis, 2002. http://library.uws.edu.au/adt-NUWS/public/adt-NUWS20030410.094714/index.html.

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Thesis (M. Sc.) (Hons.) -- University of Western Sydney, 2002.
A thesis presented to the University of Western Sydney in partial fulfilment of the rquirements for the degree of Master of Science (Honours), February, 2002. Includes bibliographical references.

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11

Hall, James Pearce. "X-ray crystallographic studies of DNA-bound polypyridyl ruthenium complexes." Thesis, University of Reading, 2014. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.658875.

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12

Barker, Nathaniel M. "The Influence of Structure in Platinum(II) Polypyridyl Polymorphic Complexes." University of Cincinnati / OhioLINK, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1627665370500068.

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13

Planas, Roure Nora. "Ruthenium polypyridyl complexes relevant to the catalytic processes in artificial photosynthesis." Doctoral thesis, Universitat Rovira i Virgili, 2011. http://hdl.handle.net/10803/33515.

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Una de les estratègies en el campde la fotosíntesis artificial consisteix en un sistema modular en que els diferents components indispensables d’un un aparell funcional són estudiats de manera independent per al seu futur acoblament. Aquesta tesi s’ha centraten la sintesis i caracterització d’una sèrie de nous compostos mono- i dinuclears de ruteni amb lligands de tipus polipiridil. S’ha estudiat l’aplicabilitat d’aquests nous compostos com a catalitzadors en processos tant importants com son l’oxidació d’ aigua a oxigen molecular i la reduccio de diòxid de carboni a àcid fòrmic. També, s’han estudiat en gran detall les propietats d’origen supramolecular detectades en els compostos dinuclears, fomentat per la directa implicació d’aquest tipus d’interaccions en els processos catalítics estudiats.
Artificial photosynthesis seeks to functionally mimik the photosynthetic process carried out by nature, and combine the energy from the sun with water to obain a “solar” fuel like hydrogen. One of the strategies in the field, consists on a modular approach in which all the components needed are studied independently, in view of their future assembly in a final operative device. This thesis has been focused on the synthesis and characterization of a series of new mono and dinuclear ruthenium componud with polylpyridylic ligands. The aplication of these new compounds as catalysts in very important processes such as water oxidation and CO2 reduction has been studied. Additionally, the suprmolecular properties detected in the dinuclear compounds has been studied in great detail, which has been promoted by the direct implication of such type of interactions in the catalytic processes studied.

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14

Howell, Sarah Louise, and n/a. "Excited state structures of polypyridyl complexes : a spectroscopic and DFT study." University of Otago. Department of Chemistry, 2005. http://adt.otago.ac.nz./public/adt-NZDU20070221.155843.

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This thesis reports the spectroscopic and computational studies of a number of Cu(I), Re(I) and Ru(II) complexes of polypyridyl ligands. The ligands considered in this study were 1,10-phenanthroline, 4,7-diphenyl-1,10-phenanthroline, 3,4,7,8-tetramethyl-1,10-phenanthroline, dibenzo[b,j][1,10]phenanthroline, dipyrido[2,3-a:3�,2�-c]phenazine, dipyrido[2,3-a:3�,2�-c]-6,7-dichlorophenazine and dipyrido[2,3-a:3�,2�-c]-6,7-dimethylphenazine. Density functional theory calculations were carried out on the polypyridyl ligands. Validation of the calculations was carried out by comparison of the predicted values to observables. The structures were compared to previously published X-ray crystal data. Calculated bond lengths were typically calculated to be within 0.02 Å of those in the crystal structure. The calculated vibrational spectra were compared to measured IR and Raman spectra. The correspondence between calculated and measured frequencies was quantified using the mean absolute deviation between the two sets of frequencies. This was typically found to be less than 10 cm⁻�. The robustness of the calculation was further tested by calculations on perdeuterated analogues of some of the ligands. The calculations were extended to metal moieties and validated as for the ligands. Resonance Raman and infrared spectra of the reduced states of some Re(I) complexes are reported. The structure and spectra have been modelled by considering the radical anion of the polypyridyl ligand and the reduced state of the complex. There is improvement in the mean absolute deviation, between calculated and observed frequencies, upon incorporation of the metal moiety into the calculation. Spectra are successfully modelled confirming the validity of the modelled structures. The resonance Raman and infrared spectra of the metal-to-ligand charge transfer excited states of some Cu(I), Re(I) and Ru(II) complexes are reported. Density functional theory calculations on the lowest energy triplet states aided in the spectral assignment of bands. Cu(I) complexes were successfully modelled with mean absolute deviations, between calculated and observed frequencies, of less than 10 cm⁻�. The spectra of the Re(I) and Ru(II) complexes were less successfully modelled. Incorporation of the Ru(II) centre into the calculation of the vibrational frequencies of dipyrido[2,3-a:3�,2�-c]phenazine complexes offers no improvement over modelling the radical anion of this polypyridyl ligand. The excited state lifetimes of a number of polypyridyl complexes have been reported. The changes in lifetimes of similar complexes were found to be consistent with the energy gap law or changes in the conjugation of the involved polypyridyl ligand. This project has allowed the excited state structures of a number of polypyridyl complexes to be determined using vibrational spectroscopy to validate density functional theory calculations. This has provided a study strategy that may be applied to other metal polypyridyl complexes.

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15

Abrahamsson, Maria. "Tuning of the Excited State Properties of Ruthenium(II)-Polypyridyl Complexes." Doctoral thesis, Uppsala : Acta Universitatis Upsaliensis, 2006. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-7230.

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16

Wolpher, Henriette. "Ruthenium(II) polypyridyl complexes in supramolecular systems relevant to artificial photosynthesis /." Stockholm : Department of Organic Chemistry, Ahrrenius Laboratory, Stockholm University, 2005. http://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-417.

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17

Bushell, Karen Lynne. "The coordination chemistry of polypyridyl ligands with secondary macrocyclic binding sites." Thesis, University of Bristol, 2000. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.301986.

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18

Willis, Kimberlee Susan. "Developing benzothiazole functionalised ruthenium(II) polypyridyl complexes as tuneable DNA binders." Thesis, Queen's University Belfast, 2014. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.675442.

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The aim of this research is to develop a range of new ruthenium(II) polypyridyl complexes to be analysed spectroscopically in the presence of calf thymus-DNA to determine their relative binding affinities to the polynucleotide, thus determining the best criteria for a detection tool for DNA. Reactions of selected functional groups on one ligand of ruthenium(II) precursor complexes lead to the synthesis of six benzothiazole containing complexes; [Ru(bpY)2(B16)]2+,, [Ru(bpy)2(P5)]2+, [Ru(phen)2(B16)]2+, [Ru (phenh(P5)]2+, [Ru(Me2bpY)2(B16)]2+ and [Ru(Me2bpy)2(P5)]2+ and four "control" complexes; [Ru (bpy)2(B2)]2+, [Ru(bpy)2(P2)] 2+, [Ru(phen)2(B2)]2+ and [Ru(phen)2(P2)]2+ bearing methyl groups. Investigation established a two-step interaction occurring between the complexes and polynucleotides, which have varying effects on the luminescence of the complexes, as a result samples were equilibrated for 24 hours before steady state measurements were recorded in the presence of DNA. Denaturation studies of DNA in the presence of each complex did not show a significant change in the melting temperature to free DNA. UV / Vis absorption spectrometry of the complexes showed variation in the absorption attributed to the benzothiazole functionalised ligand and each complex became more luminescent with increasing concentrations of DNA. The circular dichroism spectra of ct-DNA and increasing concentrations of each complex indicate that the double helical shape of the DNA is not affected as the complexes interact. From equilibrium dialysis studies with each complex it can be tentatively assigned that the ∆-enantiomer is associating most favourably with DNA. There are no significant alterations between the spectra of the methyl functionalised "control" complexes and those with increasing concentrations of DNA. Selecting the promising DNA detecting complex, [Ru(phen)2(B16)]2+ and repeating the spectroscopic studies with AT and GC rich oligos, showed the complex has a clear preference for AT rich DNA, highlighting that the preferred mode of binding at equilibrium is potentially within the minor groove of the DNA double helix.

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19

Kwong, Wai-lun, and 鄺偉倫. "Anti-cancer ytterbium porphyrin and iron polypyridyl complexes: synthesis, cytotoxicity and bioinformaticsstudies." Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 2012. http://hub.hku.hk/bib/B48521711.

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Discovery of anti-cancer cisplatin was a great success in anti-cancer chemotherapy. Numerous analogues of cisplatin such as carboplatin and oxaliplatin, were developed to improve the clinical effectiveness. Nevertheless, the clinical uses of these platinum-based drugs are limited by the occurrence of drug-resistance, narrow range of susceptible cancer types and severe toxicity. These drawbacks have stimulated the development of other metal-based compounds with distinct mechanisms of anti-cancer action. In this study, a series of ytterbium(III) porphyrin and iron(II) polypyridyl complexes were synthesized. Their anti-cancer activities were examined. With the aid of gene expression profiling and bioinformatics analysis, the mechanisms of these anti-cancer active complexes have been examined. A series of ytterbium(III) porphyrin complexes have been prepared and structurally characterized. An ytterbium(III) octaethylporphyrin complex (1) was found to exhibit potent anti-cancer activities with cytotoxic IC50 values down to sub-micromolar range. Complex (1) was shown to exist as a dimeric hydroxyl-bridged complex [Yb2(OEP)2(μ-OH)2] (where H2OEP = octylethylporphyrin) in CH2Cl2 and in solid state, and as monomeric [Yb(OEP)(DMSO)(OH)(OH2)] in DMSO/aqueous solution. Unlike various anti-cancer lanthanide complexes which are commonly proposed to target cellular DNA, our transcriptomics data, bioinformatics connectivity map analysis and cellular experiments altogether indicate that (1) exerts its anticancer effect through apoptosis which is highly associated with endoplasmic reticulum stress pathway. Two iron(II) polypyridyl complexes [Fe(qpy)(CH3CN)2](ClO4)2 (Fe-1a) (qpy =2,2’:6’,2”:6”,2’”:6”’,2””-quinquepyridine) and [Fe(Py5-OH)(CH3CN)](ClO4)2 (Fe-2a) (Py5-OH = 2,6-bis[hydroxybis(2-pyridyl)methyl]pyridine) were found to display selective cytotoxicity towards cancer cell lines over a normal lung fibroblast cell line. Affymetrix oligonucleotide microarray and bioinformatics analysis suggested that the anti-cancer mechanisms of Fe-1a and Fe-2a involve apoptosis, cell cycle arrest, activation of p53 and mitogen activated protein kinase (MAPK). Complex Fe-1a induced the formation of reactive oxygen species (ROS) in a concentration-dependent manner. Both iron complexes could cleave supercoiled plasmid DNA. The cellular DNA damage induced by both complexes was confirmed by comet assay and phospho-histone protein ( -H2AX) immunofluorescence assay. Cell cycle progression analysis revealed that Fe-1a induced both S- and G2/M-phase cell cycle arrests, whereas Fe-2a induced a G0/G1-phase arrest. Apoptosis induced by both complexes was confirmed by annexin-V/SYTOX green flow cytometry analysis and western blotting. Moreover, p53 and MAPK activation were found to be associated with the induced apoptosis. By employing the cationic porphyrin ligand, 5-(p-N-methylpyridyl)triphenylporphyrin [H2(5-MePyTPP)]+, a series of cationic metalloporphyrin complexes formulated as [M(porphyrinato)]n+ (where M = PtII, RuII, CoII or AuIII, n = 1 or 2) were prepared. The cytotoxicities of these complexes were examined. The platinum(II) and ruthenium(II) complexes were relatively non-cytotoxic towards the examined cancer cell lines with IC50 >24 μM. [CoII(5-MePyTPP)]Cl displayed a more pronounced anti-cancer activity with IC50 values between 7.48 – 17.7 μM. However, this Co(II) complex displayed poor selectivity towards the cancer cell lines compared to the normal cell line. The gold(III) porphyrin complex [AuIII(5-MePyTPP)]Cl2 showed a much higher potency (IC50 =3.01 -10.7μM) than the other [M(5-MePyTPP)]n+ prepared. By means of flow cytometry and fluorescence microscopy, [AuIII(5-MePyTPP)]Cl2 was found to induce G2/M-phase cell cycle arrest and necrotic cell death in HeLa cells.
published_or_final_version
Chemistry
Doctoral
Doctor of Philosophy

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20

Zhang, Wanji. "Dye-Sensitized Tio2 Modified with Iron Polypyridyl Catalyst for Photocatalytic Hydrogen Evolution." W&M ScholarWorks, 2016. https://scholarworks.wm.edu/etd/1477068478.

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Artificial Photosynthesis (AP) focuses on finding a way to harness solar energy to generate a chemical fuel. TiO2 semiconductors are of interest to AP research due to its relatively low cost and widespread use as an efficient charge-separating support. This research focuses on the development of a device for photocatalytic hydrogen generation. Our approach utilizes the immobilization of iron polypyridyl catalysts and ruthenium chromophores on TiO2 through stable phosphonic acid anchoring groups.

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21

Polapally, Mamatha. "Synthesis,Structure and Properties of Ruthenium Polypyridyl Metalloligand Based Metal-Organic Frameworks." TopSCHOLAR®, 2017. https://digitalcommons.wku.edu/theses/2035.

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Metal-organic frameworks (MOFs) have been extensively studied because of their amazing applications in gas storage, purification, photocatalysis, chemical sensing, and imaging techniques. Ruthenium polypyridyl complexes have been broadly considered as photosensitizers for the conversion of solar energy and photoelectronic materials. With this aspect, we have synthesized three new ruthenium polypyridyl based MOFs ([Ru(H2bpc)Cu(bpc)(Hbpc)2(H2O)]·5H2O (1), [Ru(H2bpc)(Fe(bpc)(Hbpc)2(H2O)2]·6H2O (2) and [Ru(H2bpc)Ni(bpc)(Hbpc)2(H2O)2]·6H2O (3)) from ruthenium(III) chloride, bpc (2,2’- bipyridine-4,4’-dicarboxylic acid) ligand, and 3d M(II) metal ions (M(II)= Cu(II), Fe(II), Ni(II)). These MOFs were synthesized under hydro or solvothermal conditions by using water, ethanol or methanol as solvents. The crystal structures of the new compounds contains zigzag chains of [Ru(bpc)3]n- complex ions linked by Cu, Fe or Ni complex ions individually. Above synthesized crystal structures were characterizing by single-crystal Xray and powder X-ray diffraction strategies, UV-vis and IR spectroscopy. Thermal properties were determining by thermogravimetric analysis. Magnetic properties were also studied.

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22

Borg, Anders. "Theoretical Photochemistry : Halogenated Arenes, Phytochromobilin, Ru(II)polypyridyl complexes and 6-4 photoadducts." Doctoral thesis, Uppsala universitet, Kvantkemi, 2008. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-8469.

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This thesis presents Quantum Chemical calculations on the Photochemistry of Halogenated benzenes, Phytochromobilin, Ruthenium Polypyridyl complexes and 6-4 photoadducts in DNA. The work is focused on improving the understanding of a number of experimentally observed photochemical processes in these systems. New results regarding the mechanism of photodissociation of halogenated arenes, photointerconversion of phytochromobilin are presented, as well as of the photoprocesses of Ruthenium Polypyridyl complexes and new mechanistic insights in the repair of 6-4 photoadducts in DNA.

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Ll, Yanfen. "Synthesis, Structure, and Characterization of Hybrid Solids Containing Polyoxometalates and Ruthenium Polypyridyl Complexes." TopSCHOLAR®, 2012. http://digitalcommons.wku.edu/theses/1163.

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Polyoxometalates (POMs), which are inorganic metal oxide cluster anions with discrete structures, have been extensively studied in recent years due to their large variety of applications such as medicine, biology, catalysis, material sciences and chemical analysis. Ruthenium polypyridyl complexes have been extensively studied for their applications as photosensitizers in solar energy conversion and photoelectronic materials. Recently, ruthenium heterocyclic ligand complex-based building blocks have been used for the synthesis of hybrid organic-inorganic solids through the self-assembly. We are interested in the synthesis of ruthenium polypyridyl complexes and polyoxometalate anions through different ways such as coordination bonds, hydrogen bonds and ionic bonds to form hybrid organic-inorganic solids. Here, we report four novel hybrid organicinorganic compounds, [Ru(2,2¡¦-bpy)3]2[SiW12O40] (1), [Ru(2,2¡¦- bpy)2(CH3CN)2]2[SiW12O40] (2), [Ru(2,2¡¦-bpy)3][W6O19] (3), and [Ru(2,2¡¦- bpy)3]2[Mo8O26]„ª5H2O (4) ), (2,2¡¦-bpy = 2,2¡¦-bipyridine). Compounds 1, 3, and 4 were synthesized under hydrothermal reaction methods and compound 2 was synthesized by room temperature solution method. These solids were characterized by elemental analysis, UV-vis spectroscopy, fluorescence spectroscopy, thermogravimetric analysis, IR spectroscopy, powder X-ray diffraction, and Single crystal X-ray diffraction. X-ray xii crystallographic study showed that the crystal structures of compounds 1, 2, 3 and 4 were constructed by Coulombic forces and supramolecular interactions. These molecular compounds were further connected and formed 3D structure through Cƒ{H„ª„ª„ªOPOM and other weak interactions. Spectroscopic studies demonstrated that electronic communication occurred between POMs and the sensitizers.

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24

White, Claire Michelle. "Ruthenium polypyridyl complexes designed for the non-covalent self-assembly of supramolecular systems." Thesis, University of Bristol, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.265497.

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Prusakova, Valentina. "The Design, Syntheses, and Photophysics of Novel Pt(II) Polypyridyl Arylacetylides and Arylthiolates." Bowling Green State University / OhioLINK, 2012. http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1354731350.

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26

Sun, Yujie. "Ru(II) and Os(II) Polypyridyl Complexes as Luminescence Sensors and PDT Agents." The Ohio State University, 2010. http://rave.ohiolink.edu/etdc/view?acc_num=osu1279227020.

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Wang, Lei. "Ultrafast Excited State Investigation of Ruthenium and Osmium Polypyridyl SulfoxideComplexes and BOPHY Dyes." Ohio University / OhioLINK, 2015. http://rave.ohiolink.edu/etdc/view?acc_num=ohiou1433864223.

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Loftus, Lauren Marie. "Tuning the Excited States and Reactivity of Polypyridyl Ru(II) Complexes for Photochemotherapy." The Ohio State University, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=osu156579728991504.

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Race, Nicholas. "Iron Polypyridyl Catalysts Assembled on Metal Oxide Semiconductors for Heterogeneous Photocatalytic Hydrogen Generation." W&M ScholarWorks, 2018. https://scholarworks.wm.edu/etd/1530192812.

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Artificial Photosynthesis (AP) provides a promising method for the conversion of solar energy to chemical fuel in the form of H2 and O2. Development of heterogeneous systems in which H2 evolution catalysts are immobilized on metal oxide semiconductors is imperative for the large-scale implementation of AP systems. This research focuses on the immobilization of an active H2 evolution catalyst on large band gap semiconductors for the development and optimization of a highly active photocatalytic H2 generation system.

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30

Walsh, Penelope Jane, and n/a. "Modelling and spectroscopy of polypyridyl and porphyrin complexes for electroluminescence and solar cell applications." University of Otago. Department of Chemistry, 2007. http://adt.otago.ac.nz./public/adt-NZDU20070927.151236.

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This thesis reports the spectroscopic and computational studies of two classes of compounds, which have applications in new optoelectronic materials technology. Substituted ligands of dipyrido-[3,2a:2�,3�c]phenazine (dppz), and their Cu(I), Re(I) and Ru(II) complexes have utility in organic electroluminescent devices. A series of Zn(II) tetraphenylporphyrins with conjugated functional groups at the β-position have been used with success in liquid heterojunction dye-sensitized solar cells. The vibrational spectra and optoelectronic properties of the two classes were investigated using Raman, resonance Raman and transient resonance Raman spectroscopy, in conjunction with density functional theory methods. Density functional theory frequency calculations were used to aid vibrational mode assignments for the dppz compounds, and show close agreement with the experimental non-resonance Raman spectra. The enhancement of modes which are localized on differing sections of the ligand was identified. The nature of the absorbing chromophores for the dppz ligands and complexes was established using resonance Raman spectroscopy in concert with vibrational assignments from calculations. Transient resonance Raman spectra of the ligands provided spectral signatures for the triplet ligand-centred state; these features were observed in the TR� spectra of the metal complexes, along with other features attributable to MLCT states. Electroluminescent devices were fabricated using the dppz ligands and complexes as emissive dopants, and their properties investigated. The optoelectronic behaviour of the devices was found to be influenced by the mechanism of exciton formation on the dopant. The device properties were also dependent on the dopant concentration, the concentrations of other components and the driving voltage. The electronic structure of the porphyrin compounds was investigated using time-dependent density functional theory methods. Comparison of calculated optical transitions with experimental data shows that the calculations predict trends in the optical absorption spectra with change of functional group and with increase in conjugation chain length. The calculations suggest that the electron-withdrawing substituent decreases the configuration interaction effect by breaking the degeneracy of the two lowest unoccupied MOs, and other configuration interaction effects come into play involving other frontier MOs. Interrupting the conjugation of the functional group is shown to mitigate the breakdown of the configuration interaction. The perturbation of the normal electronic structure of the porphyrin by the substituent was also investigated using resonance Raman spectroscopy. Vibrational analysis identified bands due to the substituent, implying coupling between the porphyrin and substituent chromophores. Changes in frequency of porphyrin core modes due to the differing substituents and different metal centres were reproduced by density functional theory calculations. This project has allowed the spectroscopic investigation of the active optical states in a number of polypyridyl and porphyrin compounds, and determined the efficacy of DFT and TDDFT calculations to predict the properties of these compounds.

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31

Steen, Robert. "The Synthesis of Molecular Switches Based Upon Ru(II) Polypyridyl Architecture for Electronic Applications." Licentiate thesis, Västerås : Department of Biology and Chemical Engineering, Mälardalen University, 2007. http://urn.kb.se/resolve?urn=urn:nbn:se:mdh:diva-356.

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32

Lazarides, Theodore. "Luminescent d-block metal polypyridyl complexes bearing secondary macrocyclic or non-macrocyclic binding sites." Thesis, University of Sheffield, 2005. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.427184.

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33

Lanquist, Austin Paul. "Investigation of Ligand Electronic Effects on the Photodissociation of Acetonitrile from Ruthenium Polypyridyl Complexes." The Ohio State University, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=osu152570510019408.

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34

Olaprath, Waynie Wilson. "Electrochemical and spectroscopic characterization of a polypyridyl Ru(II) complex containing a fused alloxazine /." View online, 2009. http://repository.eiu.edu/theses/docs/32211131598949.pdf.

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35

Majewski, Marek B. "Ruthenium(II) complexes bearing polypyridyl ligands with amide bound thienyl groups for photochemical energy conversion." Thesis, University of British Columbia, 2013. http://hdl.handle.net/2429/44478.

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36

Mengel, Andreas K. C. [Verfasser]. "Bis(tridentate) polypyridyl transition metal complexes for DSSC and LEC applications / Andreas K. C. Mengel." Mainz : Universitätsbibliothek Mainz, 2017. http://d-nb.info/1139215035/34.

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37

Tart, Nicholas Michael. "Photophysical properties of iradium(III) and ruthenium(II) complexes containing bis- and terdentate polypyridyl ligands." Thesis, University of Sheffield, 2010. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.527229.

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38

尹俊偉 and Chun-wai Wan. "Spectroscopic properties and coordination chemistry of d10 metal complexes with the polypyridyl and naphthyridyl ligands." Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 2000. http://hub.hku.hk/bib/B31223564.

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39

Folmar, Michele L. "Synthesis and Characterization of a New Ruthenium(II) Polypyridyl Compound with a Quinolate-Type Ligand." The Ohio State University, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=osu1469047981.

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40

Evans, Alba Pilar. "New Ruthenium(II) Polypyridyl Compounds with Quinoline Type Ligands for the Treatment of Cutaneous Leishmaniasis." The Ohio State University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=osu1511881725973833.

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41

Margonis, Caroline Marie. "Polyaromatic-Terminated Iron Polypyridyl Complexes For The Functionalization Of Carbon Surfaces And Electrocatalytic Hydrogen Generation." W&M ScholarWorks, 2021. https://scholarworks.wm.edu/etd/1627047877.

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Artificial Photosynthesis (AP) focuses on developing methods for the conversion of solar energy into chemical fuel in the form of H2 and O2. Heterogeneous photocatalytic systems incorporating carbon nanotubes (CNTs) have shown much promise but are currently limited and expensive due to their reliance on noble metals. To that end, this work focuses on the development and synthesis of cheaper naphthalene- and pyrene-terminated iron polypyridyl complexes for use in the simultaneous functionalization of carbon surfaces, electrocatalytic proton reduction, and eventual incorporation in photocatalytic systems. Cyclic voltammetry was used to characterize the adsorption behavior of each complex on the surface of a glassy carbon electrode. For the naphthalene variant, electrode-surface adsorption saturation was reached after 720 minutes with a maximum surface coverage of 7.7*10-11 mol/cm2, and the complex was found to be relatively surface-stable in solvents lacking hydrogen-bond donors or acceptors. Upon the addition of TFA, proton reduction catalysis occurred at -1.13 V vs. SCE in CH3CN with an overpotential of 480 mV. Additionally, the surface adsorbed naphthalene-functionalized complex was found to be active for hydrogen generation from purely aqueous buffer solutions of pH = 3.8 – 6.2. A pyrene variant was synthesized through a palladium-catalyzed amination. Its maximum surface coverage on a glassy carbon electrode was found to be 3.9*10-11mol/cm2. The complex was found to be a weak electrocatalyst for proton reduction, with proton reduction catalysis occurring at -1.00 V vs. SCE upon the addition of TFA.

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42

Wan, Chun-wai. "Spectroscopic properties and coordination chemistry of d10 metal complexes with the polypyridyl and naphthyridyl ligands /." Hong Kong : University of Hong Kong, 2000. http://sunzi.lib.hku.hk/hkuto/record.jsp?B22227301.

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43

Sun, Yang. "STUDY OF THE MECHANISM OF ACTION FOR Ru(II) POLYPYRIDYL COMPLEXES AS POTENTIAL ANTICANCER AGENTS." UKnowledge, 2018. https://uknowledge.uky.edu/chemistry_etds/97.

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Application of chemotherapeutic agents in current cancer treatment has been limited by adverse effects as poor selectivity results in systemic toxicity; most chemotherapy approaches also experience inherited or acquired drug resistance which lead to reduced treatment outcome. Research efforts have focused on the discovery of novel chemotherapies that overcome the limitations mentioned above. Ru(II) polypyridyl complexes with anti-cancer properties have been extensively studied as traditional cytotoxic agents and photodynamic therapy agents due to their photophysical and photochemical characteristics. Most research has focused on the design of Ru(II) polypyridyl complexes that have affinities to nucleic acids as inspired by the classic small molecule metal complex cisplatin. Though modifying the structures of ligands on the ruthenium metal center, the hydrophilicity, charge state and photochemical properties can be tuned, resulting to Ru(II) polypyridyl complexes that act through cellular targets other than DNA. Understanding the mechanism of action and identifying functional targets remain the challenging and complex research topic in the design and study of novel medication or candidates. With the development of semi-high throughput cytological profiling in a bacterial system, rapid investigation of the mechanism of action can be achieved to distinguish anti-cancer agents which possess different mechanisms of actions. Ru(II) polypyridyl complexes with different scaffolds have been studied and suggested to have anti-cancer properties through DNA damage response, and/or translational inhibition.

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44

Jäger, Michael. "Beyond Classical Ruthenium(II) Polypyridyl Complexes : Photosensitizers as Building Blocks For Linear Donor-Photosensitizer-Acceptor Assemblies." Doctoral thesis, Uppsala universitet, Institutionen för fotokemi och molekylärvetenskap, 2009. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-9555.

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This thesis describes ruthenium(II) polypyridyl-type complexes tailored for artificial photosynthesis. Inspired by Nature, the primary events in photosystem II are mimicked by donor-photosensitizer-acceptor (D-P-A) assemblies. The photosensitizer plays a key role in such processes, and the combination of structural and photophysical properties is essential to control the electron transfer steps. In the first part, the general requirements for photosensitizers are discussed. The second part deals with [Ru(bpy)3]2+-benzoquinone (Q) dyads (bpy is 2,2´-bipyridine) based on an asymmetric 5,5´-bisamide substituted bpy. Rapid electron-transfer from the excited state is observed to generate the RuIII-Q- charge separated states but preliminary results show no effect of the directionality of the amide link. In the main part, a strategy to overcome the photophysical limitations of RuII bistridentate complexes (e.g. [Ru(tpy)2]2+, tpy is 2,2´:6´,2´´-terpyridine) is explored. The prototypical [Ru(dqp)2]2+ complex (dqp is 2,6-di(quinolin-8-yl)pyridine) is synthesized which displays a 3000 ns excited state lifetime at room temperature, reversible redox chemistry and high photostability. The synthesis of 4-substituted dqp is achieved via SUZUKI coupling using 8-quinoline boronic acid or ring-formation of the central pyridine. A markedly rich Ru coordination chemistry was observed, e.g. facial and meridional isomers of [Ru(dqp)2]2+. Using a chloride-free [Ru(dqp-R)(MeCN)3]2+ intermediate allows the synthesis of heteroleptic meridional [Ru(dqp-R)(dqp-R’)]2+ (R,R’ = -H, -CO2Et, -NH2, -OMe, -Br, -PhBr, …) in high yields. The meridional complexes show long-lived luminescence (450 - 5500 ns) and reversible redox chemistry. The photochemical reactivity has been investigated in typical electron-transfer reactions, e.g. in a supramolecular P-A dyad and in a multimolecular approach using biomimetic components (Mn and Fe complexes). The dqp ligand is further used to synthesize FeII, RhIII, cyclometallating RuII complexes and an aza-analogue of [Ru(dqp)2]2+ and is discussed in the final part. These complexes were prepared with the aim to further tune the redox properties while maintaining good photophysical properties.

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唐偉方 and Wai-fong Tong. "X-ray crystallographic studies of osmium and ruthenium complexes of multianionic, polypyridyl and tertiary amine ligands." Thesis, The University of Hong Kong (Pokfulam, Hong Kong), 1991. http://hub.hku.hk/bib/B31210016.

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46

Tong, Wai-fong. "X-ray crystallographic studies of osmium and ruthenium complexes of multianionic, polypyridyl and tertiary amine ligands /." [Hong Kong : University of Hong Kong], 1991. http://sunzi.lib.hku.hk/hkuto/record.jsp?B13019272.

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47

Rohrabaugh, Thomas Nelson Jr. "The Application of Ru(II) Polypyridyl Photoinduced Ligand Exchange from Drug Delivery to Photoactivation of Fluorescent Dyes." The Ohio State University, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=osu1533226287168103.

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48

Ono, Takashi. "Second-Row Transition-Metal Complexes Relevant to CO2." Doctoral thesis, Universitat Rovira i Virgili, 2014. http://hdl.handle.net/10803/276964.

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dinucleares de rutenio que contienen ligandospolypyridyl. Estos complejos se han aplicado para las reacciones catalíticas, tales como la reducción de CO2 y la oxidación del agua y sustrato orgánico. En la primera, las actividades catalíticas hacia la reducción de CO2 se han investigado desde el punto de vista de las propiedades electrónicas y estéricas de los catalizadores, así como su nuclearidad. En el segundo, la aplicación de mono-y dinucleares complejos de Ru-aqua que contienen ligando tridentadoaniónico hacia reacción de oxidación se ha estudiado. Además, una reactividad potencial de dianión molibdato, que puede ser considerado como modelo homogéneo de catalizadores de óxido de metal heterogéneos para la transformación de CO2 se ha estudiado.
This thesis has been focused on the synthesis and characterization of a series of new mono- and dinuclear ruthenium complexes containing polypyridyl ligands. These complexes have been applied for the catalytic reactions, such as CO2 reduction and oxidation of water and organic substrate. In the first, the catalytic activities toward CO2 reduction have been investigated from the viewpoint of electronic and steric properties of the catalysts as well as their nuclearity. In the second, the application of mono- and dinuclear Ru-aqua complexes containing anionic tridentate ligand toward oxidation reaction has been studied. Additionally, a potential reactivity of molybdate dianion, which can be considered as homogeneous model of heterogeneous metal oxide catalysts for CO2 transformation has been studied.

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49

Kender, William Theodore. "Controlling Excited State Electron Delocalization via Subtle Changes to Inorganic Molecular Structures." The Ohio State University, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=osu1534271989190317.

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50

Lundqvist, Maria J. "Quantum chemical modeling of dye-sensitized titanium dioxide : ruthenium polypyridyl and perylene dyes, TiO₂ nanoparticles, and their interfaces /." Uppsala : Acta Universitatis Upsaliensis, 2006. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-7141.

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