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King, Jennifer L. "Organometallic chemistry in supercritical fluid solution." Thesis, University of Nottingham, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.262952.
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King, Hannah Elizabeth. "Effect of Solution Chemistry on Schwertmannite Formation." Thesis, Virginia Tech, 2015. http://hdl.handle.net/10919/54028.
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Natural nanominerals are abundant in Earth's critical zone and important in innumerable environmental processes that affect water quality. The chemical behavior of many natural nanominerals is related to their extreme small size (<10 nm) and high surface area. Atomic structural and chemical heterogeneity are also important factors affecting nanoparticle reactivity, and are a consequence of the mechanisms and complex (natural) conditions by which they form. The relationships between these factors remain poorly understood and limit our ability to predict the formation, transformation, and chemical behavior of natural nanominerals in the environment.
We are using a poorly crystalline ferric hydroxysulfate nanomineral, schwertmannite, as a model system to understand the effect of formation conditions, specifically solution chemistry, on its physico-chemical characteristics. Previous studies indicate schwertmannite has highly variable bulk sulfate (Fe/S molar from 3-15) and water contents (Caraballo et al., 2013). In addition, both natural and synthetic schwertmannites have recently been described as "polyphasic" (i.e., consisting of sulfate-poor, goethite-like ordered domains embedded in a sulfate-rich, amorphous material) from observations using transmission electron microscopy (French et al., 2012). We hypothesize that solution chemistry at the time of schwertmannite formation directly affect its composition and structure.
Using a factorial experiment design, we investigated the effects of increasing solution sulfate concentration ([SO4]/[Fe] at 1, 2, 3 and 5) and pH (2.4-5.6) on the crystallinity and composition of the products. Ferric hydroxide and hydroxysulfate solids were precipitated in batches by the rapid oxidation of Fe(II) by hydrogen peroxide, similar to what is seen in natural environmental systems. Sulfate and hydroxide concentrations were varied by addition of NaSO4 and NaOH, respectively. Solids were characterized using synchrotron X-ray diffraction (XRD), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), inductively coupled plasma-mass spectrometry (ICP-MS), scanning electron microscopy (SEM), and high resolution- transmission electron microscopy (HR-TEM). Our results show that schwertmannite is the only precipitate formed at low pH and that goethite rapidly becomes dominant at pH > 3.5. High-resolution TEM showed our synthetic schwertmannite samples consist of poorly crystalline goethite-like nanodomains within an amorphous solid, similarly seen in previous results. ICP-MS results reveal a narrow Fe/S molar ratio of 4.5 ±0.1 for our synthetic schwertmannite, which suggests that schwertmannite chemical composition does not depend strongly on pH or initial solution sulfate concentration. Increasing pH from 2.4 to 3.2 also has little effect on the crystallinity, bulk Fe/S ratio and water contents of schwertmannite. Increasing solution [SO4]/[Fe] also has little to no impact on crystallinity, water content or the amount of sulfate incorporated in schwertmannite. Thus, schwertmannite crystallinity and composition is not affected by initial solution sulfate and concentration under our experimental conditions.
Thermal analysis allows us to independently measure OH and SO4 content in synthetic schwertmannite. In doing so, we propose a more accurate chemical formula (Fe8Oz(OH)24-2z-2x(SO4)x). The average stoichiometry based on thermal analysis of schwertmannite precipitated at [SO4]/[Fe] = 1 and pH ranging from ~2.4 2.9 is Fe8O6.51(OH)8.4(SO4)1.28. Interestingly, the calculated number of moles of oxygen is less than 8, which suggests that the standard formula Fe8O8(OH)8-2x(SO4)x is incorrect. These results for synthetic samples provide important constraints for future studies aimed at better understanding the formation, compositional variability and chemical behavior of natural schwertmannite.Master of Science
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Silvester, Debbie Sue. "Electrochemical studies in room temperature ionic liquids." Thesis, University of Oxford, 2008. http://ora.ox.ac.uk/objects/uuid:be9e6269-f19a-48de-96e3-41c0c7143d6a.
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The work presented in this thesis involves the application of room temperature ionic liquids (RTILs) as solvents for use in electrochemical experiments. Initially, the fundamentals of electrochemistry is presented, followed by a comprehensive overview of RTILs in terms of their properties, applications and their behaviour as electrochemical solvents compared to conventional aprotic solvents. The results of 8 original studies are then presented as follows: X-Ray photoelectron spectroscopy is used to quantify the concentration of bromide ions in an ionic liquid, and is independently confirmed by potential-step chronoamperometry. The reaction mechanisms and kinetics for the electrochemical reduction of some aromatic nitro compounds (namely nitrobenzene and 4-nitrophenol) are determined. The electrochemistry of phosphorus trichloride and phosphorus oxychloride is studied in detail for the first time, due to the unusual stability of these highly reactive compounds in RTILs. The reductions and oxidations of sodium and potassium nitrate are studied, giving rise to 'melt'-like behaviour. The electrodeposition of sodium oxide on platinum is also demonstrated. The electrochemical oxidation of nitrite and the oxidation and reduction of the toxic gas, nitrogen dioxide, is presented. The oxidation of hydrogen gas is studied in ten RTILs with a range of different cations and anions, and contrasting interactions with the RTIL anions are seen. The electrochemical oxidation of ammonia gas is studied in five RTILs with different anions and a general reaction mechanism is suggested. The reduction of benzoic acid is studied in six RTILs, and the kinetics of the dissociation step are found to be very fast. The first five studies are all carried out in one particular ionic liquid, and the reactions and mechanisms are compared to that observed in conventional aprotic solvents. The last three studies employ several RTILs with different cations and anions to look at the contrasting interaction of protons with the RTIL cation/anion and ultimately help to understand the pH properties of the solvent. The overall findings from the work in this thesis are that some reactions and mechanisms (e.g bromide, nitro derivatives and ammonia) are generally the same in RTILs as in conventional aprotic solvents, but other species (e.g. nitrates, phosphorus derivatives) show remarkably different behaviour. It has also been demonstrated that RTILs are suitable media for the detection of nitrogen dioxide, hydrogen and ammonia gases. This suggests that RTILs could potentially offer many advantages when employed as solvents in electrochemical reactions and in amperometric gas sensors.
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Lelli, Moreno. "Solution Structure and Solution Dynamics in Chiral Ytterbium(III) Complexes." Doctoral thesis, Scuola Normale Superiore, 2007. http://hdl.handle.net/11384/85804.
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Lough, Julie Ann. "Aqueous solution chemistry of ruthenium arene anticancer complexes." Thesis, University of Warwick, 2010. http://wrap.warwick.ac.uk/35524/.
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Metal complexes currently are currently of much interest in the field of anticancer drug development. Platinum complexes such as cisplatin, are now widely used in the clinic and have led to a focus on the synthesis of new classes of other metal-based complexes, such as ruthenium anticancer drugs. In order to understand the mechanism of action of these complexes and to improve structureactivity relationships thereof, a comprehensive study of the solution chemistry is important. In this thesis the mechanism and kinetic detail of the exchange of amino protons on one such class of complex, [(η6-biphenyl)Ru(N,N’- ethylenediamine)Cl]+ was investigated in detail. Stereospecific assignment of NH protons was carried out by NOESY NMR on a pyridine adduct [(η6- biphenyl)Ru(N,N’-ethylendiamine)(N-pyridine)]2+. Using 1H and 2H NMR spectroscopy, rates of exchange were observed at different pH values, temperatures and ionic strengths a series of N-H/2H exchange reactions were studied and the data collected. The data are consistent with an exchange mechanism involving proton abstraction from the amine, followed by favourable reprotonation on the lowerface (relative to the overhanging arene) of the Ru(N,N’- ethylendiamine) five membered ring. In chlorido complexes this leads to the exchange of lower proton at a rate of three times that of those on the upperface at 298 K. To investigate the effects of electron density on the ruthenium on the exchange rates a series of π-donor pyridine ligands (pyridine, 4-methylpyridine, 4- tert-butylpyridine, and 4-methoxypyridine) in the place of the chloride were studied. The exchange rates were also investigated and showed a correlation between the basicity of the pyridine derivative and the favourability of exchange on the lower face, increasing this bias upto 11 fold. Density functional theory calculations suggests that there is an overlap between the p-orbital of the (ethylenediamine) nitrogen and the π*-antibonding orbital on the Ru-N(Pyridine) bond and σ*- antibonding orbital on the Ru-Cl bond, in their respective complexes. This overlap is proposed as a stabilising force on the deprotonated nitrogen allowing for a negative charge to be more stabile in one lobe of the p-orbital preferential to another. Following abstraction of the proton, the lone pair on the nitrogen is stabilised by an antibonding orbital, the top face less is susceptible to proton addition. Since DNA is a potential target for these complexes, the changes in shape induced by metal binding were investigated using Ion-Mobility Mass Spectrometry for the first time. Also in this work, the first ion-mobility mass spectrometry studies of the collisional cross sections (CCSs) of small complexes (<100 Å2) is also presented. This was developed using a new glycine based calibrant. Following binding of [(η6-biphenyl)Ru(N,N’- ethylenediamine)Cl]+ to the DNA hexamer d(CACGTG) changes in CCS values between ruthenated and non-ruthenated hexamers were studied. The change in CCS between these was not additive and suggestive of some folding or intercalation occurring upon ruthenium binding. Finally, attempts were madeto investigate shape change induced in DNA by binding to cisplatin using Förster Resonance Energy Transfer Methods are described. To date these results are inconclusive but work in this field is ongoing.
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Clarke, Matthew J. "Chemistry and spectroscopy in supercritical and polymer solution." Thesis, University of Nottingham, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.307843.
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Palmer, J. W. "The solution chemistry of magnetite and mild steel." Thesis, University of Nottingham, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.371288.
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Dimmock, Paul W. "Aqueous solution chemistry of mixed-metal cluster complexes." Thesis, University of Newcastle Upon Tyne, 1990. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.278725.
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Oulabi, M. "A spectroscopic study of uranium(IV) solution chemistry." Thesis, University of Surrey, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.235365.
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Patel, A. "Aqueous solution chemistry of molybdenum tungsten and ruthenium." Thesis, University of Stirling, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.233793.
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Da, Silva Rodrigues Rafael Alexandre. "Dynamic covalent chemistry at the solution: Surface interface." Thesis, Queensland University of Technology, 2020. https://eprints.qut.edu.au/200450/1/Rafael_Da%20Silva%20Rodrigues_Thesis.pdf.
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Mechanically interlocked architectures have shown great promise in applications such as catalysis, sensing and drug delivery. They have also been developed as the basis of molecular machinery. However, the use such systems often requires their incorporation to surfaces or solid supports for amplified concerted action and reusability. This research investigated new methods for the attachment of rotaxanes to polymer resins. By adopting a dynamic covalent approach to surface attachment, great improvements in proportion of rotaxanes, when compared to kinetic by-products, were achieved on polymer resins.
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Eriksson, Margareta. "Ozone chemistry in aqueous solution : ozone decomposition and stabilisation." Licentiate thesis, Stockholm, 2005. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-303.
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Chilton, R. A. "Gas release and solution." Thesis, University of Leeds, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.234082.
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Zhang, Jingtao. "Solution Phase Route towards Titanium Carbide." The Ohio State University, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=osu1563391108014095.
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Li, Xin. "Applications of Molecular Dynamics in Atmospheric and Solution Chemistry." Doctoral thesis, KTH, Teoretisk kemi och biologi, 2011. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-33309.
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This thesis focuses on the applications of molecular dynamics simulation techniques in the fields of solution chemistry and atmospheric chemistry. The work behind the thesis takes account of the fast development of computer hardware, which has made computationally intensive simulations become more and more popular in disciplines like pharmacy, biology and materials science. In molecular dynamics simulations using classical force fields, the atoms are represented by mass points with partial charges and the inter-atomic interactions are modeled by approximate potential functions that produce satisfactory results at an economical computational cost. The three-dimensional trajectory of a many-body system is generated by integrating Newton’s equations of motion, and subsequent statistical analysis on the trajectories provides microscopic insight into the physical properties of the system. The applications in this thesis of molecular dynamics simulations in solution chemistry comprise four aspects: the 113Cd nuclear magnetic resonance shielding constant of aqua Cd(II) ions, paramagnetic 19F nuclear magnetic resonance shift in fluorinated cysteine, solvation free energies and structures of metal ions, and protein adsorption onto TiO2. In the studies of nuclear magnetic resonance parameters, the relativistic effect of the 113Cd nucleus and the paramagnetic shift of 19F induced by triplet O2 are well reproduced by a combined molecular dynamics and density functional theory approach. The simulation of the aqua Cd(II) ion is also extended to several other monovalent, divalent and trivalent metal ions, where careful parameterization of the metal ions ensures the reproduction of experimental solvation structures and free energies. Molecular dynamics simulations also provided insight into the mechanism of protein adsorption onto the TiO2 surface by suggesting that the interfacial water molecules play an important role of mediating the adsorption and that the hydroxylated TiO2 surface has a large affinity to the proteins. The applications of molecular dynamics simulations in atmospheric chemistry are mainly focused on two types of organic components in aerosol droplets: humic-like compounds and amino acids. The humic-like substances, including cis-pinonic acid, pinic acid and pinonaldehyde, are surface-active organic compounds that are able to depress the surface tension of water droplets, as revealed by both experimental measurements and theoretical computations. These compounds either concentrate on the droplet surface or aggregate inside the droplet. Their effects on the surface tension can be modeled by the Langmuir-Szyszkowski equation. The amino acids are not strong surfactants and their influence on the surface tension is much smaller. Simulations show that the zwitterionic forms of serine, glycine and alanine have hydrophilic characteristics, while those of valine, methionine and phenylalanine are hydrophobic. The curvature dependence of the surface tension is also analyzed, and a slight improvement in the Köhler equation is obtained by introducing surface tension corrections for droplets containing glycine and serine. Through several examples it is shown that molecular dynamics simulations serve as a promising tool in the study of aqueous systems. Both solute-solvent interactions and interfaces can be treated properly by choosing suitable potential functions and parameters. Specifically, molecular dynamics simulations provide a microscopic picture that evolves with time, making it possible to follow the dynamic processes such as protein adsorption or atmospheric droplet formation. Moreover, molecular dynamics simulations treat a large number of molecules and give a statistical description of the system; therefore it is convenient to compare the simulated results with experimentally measured data. The simulations can provide hints for better design of experiments, while experimental data can be fed into the refinement of the simulation model. As an important complementary to experiments, molecular dynamics simulations will continue to play significant roles in the research fields of physics, chemistry, materials science, biology and medicine.QC 20110511
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Ooi, B. L. "Aqueous solution chemistry of molybdenum and tungsten cluster complexes." Thesis, University of Newcastle Upon Tyne, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.383985.
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Chen, Feng. "Molecular dynamics simulations of solution mixtures and solution/vapor interfaces." Diss., Manhattan, Kan. : Kansas State University, 2010. http://hdl.handle.net/2097/2421.
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Roberts, Kevin Edward. "Precipitation of neptunium dioxide from aqueous solution." Scholarly Commons, 1999. https://scholarlycommons.pacific.edu/uop_etds/2682.
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Tens of thousands of metric tons of highly radioactive, nuclear waste have been generated in the United States. Currently, there is no treatment or disposal facility for these wastes. Of the radioactive elements in high-level nuclear waste, neptunium (Np) is of particular concern because it has a long half-life and may potentially be very mobile in groundwaters associated with a proposed underground disposal site at Yucca Mountain, Nevada. Aqueous Np concentrations observed in previous, short-term solubility experiments led to calculated potential doses exceeding proposed long-term regulatory limits. However, thermodynamic data for Np at 25°C showed that these observed aqueous Np concentrations were supersaturated with respect to crystalline NpO 2 . It was hypothesized that NpO 2 is the thermodynamically stable solid phase in aqueous solution, but it is slow to form in an aqueous solution of NpO 2 + on the time scale of previous experiments. The precipitation of NpO 2 would provide significantly lower aqueous Np concentrations leading to calculated doses below proposed regulatory limits. To test this hypothesis, solubility experiments were performed at elevated temperature to accelerate any slow precipitation kinetics. Ionic NpO 2 + (aq) was introduced into very dilute aqueous solutions of NaCl with initial pH values ranging from 6 to 10. The reaction vessels were placed in an oven and allowed to react at 200°C until steady-state aqueous Np concentrations were observed. In all cases, aqueous Np concentrations decreased significantly from the initial value of 10 −4 M. The solids that formed were analyzed by x-ray powder diffraction, x-ray absorption spectroscopy, and scanning electron microscopy. The solids were determined to be high-purity crystals of NpO 2 . This is the first time that crystalline NPO 2 has been observed to precipitate from NpO 2 + (aq) in near-neutral aqueous solutions. The results obtained demonstrate that Np will precipitate as NpO 2 in aqueous solutions thereby leading to significantly lower aqueous Np concentrations.
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Liang, Zihao. "The Solution Behavior of Macroions Regulated by Host-Guest Chemistry." University of Akron / OhioLINK, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=akron152225667682411.
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Razzaghi, Mortezaali. "Quantum Tunneling in Hydride Transfer Reactions in Solution." Thesis, Southern Illinois University at Edwardsville, 2014. http://pqdtopen.proquest.com/#viewpdf?dispub=1549836.
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The secondary kinetic isotope effects for the hydride transfer reactions from aliphatic alcohols to four carbocations (NAD+ models) in acetonitrile were determined. The results suggest that the hydride transfer takes place by tunneling and that the rehybridizations of both donor and acceptor carbons lag behind the H-tunneling. This is quite contrary to the observations in alcohol dehydrogenases where the importance of enzyme motions in catalysis is manifested.
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Chen, Rui. "HIGH PERFORMANCE SOLUTION-PROCESSED PEROVSKITE PHOTOVOLTAICS BY NOVEL MATERIALS." University of Akron / OhioLINK, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=akron1617818409646272.
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Mokoena, Allistair Frans. "Water dynamics about selected monosaccharides in solution." Master's thesis, University of Cape Town, 2014. http://hdl.handle.net/11427/13382.
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Includes bibliographical references.The solubility of molecules in water is governed, amongst other things, by the inherent properties of the solute molecules and water molecules. Water molecules are able to simultaneously form hydrogen bonds as donors and acceptors and thus have unique properties as solvent molecules. These properties influence how water interacts with solute molecules. The mechanism of hydrogen bond exchange plays a role in the hydration of solute molecules. A key to understanding some of the biological processes lies in understanding how solutes interact with water. In this thesis, the hydration of monosaccharides has been studied using computational methods. The hydration structure is elucidated by pair distribution functions and spatial distribution functions. Hydrogen bond exchange dynamics were investigated on the basis of the molecular jump mechanism. Evaluation of the hydrogen bond exchange dynamics reveals two possible pathways. The first pathway corresponds to the molecular jump mechanism reported in literature. The second pathway is described. This pathway provides details on the water-hydroxyl interactions taking place around the monosaccharides. It is shown that the presence of a primary alcohol on pyranose based molecules induces a configuration that allows favourable interactions between water molecules and hydroxyl groups on the sugar molecules. A region of high water density is formed between the primary alcohol, ring oxygen and the hydroxyl on the anomeric carbon. This is due to rotations by water molecules from one hydroxyl, to the adjacent hydroxyl on the sugar molecule. It is not only the presence of the primary alcohol that plays a role in the hydration of the monosaccharides. The relative position of the hydroxyl on the anomeric carbon is shown to create a topology conducive of hydroxyl to hydroxyl hydrogen bond exchanges. The hydration of monosaccharides is rationalised by these effects.
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Wang, Ruifu. "The Solution Behavior of Abundant Metals based Water Oxidation Catalysts." University of Akron / OhioLINK, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=akron1460301627.
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Baxter, Rodney Charles. "The thermodynamics of binary liquid mixtures of compounds containing multiple bonds." Thesis, Rhodes University, 1989. http://hdl.handle.net/10962/d1016079.
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Excess thermodynamic properties have been determined for several binary liquid mixtures with the aim of testing various thermodynamic theories and postulates. Excess molar enthalpies, HEm, have been determined using an LKB flow microcalorimeter and excess molar volumes, VEm, have been determined using an Anton Paar vibrating tube densitometer. The activity coefficients at infinite dilution ƴ∞₁₃, have been determined using an atmospheric pressure gas-liquid chromatograph. The excess molar enthalpies and the excess molar volumes have been measured at 298.15 K for systems involving the bicyclic compounds decahydronaphthalene (decalin), 1,2,3,4-tetrahydronaphthalene (tetralin), bicyclohexyl, or cyclohexylbenzene mixed with 1- hexene, 1-hexyne, 1-heptene, 1-heptyne, cyclohexene, 1,3-cyclohexadiene, 1,4- cyclohexadiene, or benzene. These excess properties have also been measured for systems where the bicyclic compound has been replaced with benzene, cyclohexane or n-hexane. The results show defmite trends related to the size, shape, and the degree of unsaturation of the component molecules. The Flory theory has been used to predict excess molar enthalpies and excess molar volumes for {(a bicyclic compound or benzene or cyclohexane or n-hexane) +(an n-alkane or a 1-alkene or a 1-alkyne or a cycloalkane or cyclohexene or a cycloalkadiene or benzene)}. The one parameter equations offer reasonably good correlations between the predicted and the experimental results. More insight into the origins of the contnbutions to the excess thermodynamic properties for these systems has been gained by considering the approximate equations of Patterson and co-workers, which separate the interactional and the free volume contributions to the excess molar enthalpy and the excess molar volume. The one parameter equations have adequately rationalized a good deal of the observed behaviour for HEm and VEm. The theory of Liebermann and co-workers, which does not employ any adjustable parameters, has not been as successful at predicting the excess thermodynamic properties for the above systems. The activity coefficients at infinite dilution have been measured at 278.15 K, 288.15 K and 298.15 K for n-bexane, 1-bexene, 1-hexyne, n-heptane, 1-heptene, 1-heptyne, cyclohexane, cyclohexene, 1,3-cyclohexadiene, 1,4-cyclohexadiene, and benzene, in decalin, tetralin, bicyclohexyl, and cyclohexylbenzene. Solvent losses from the column have been accounted for by an extrapolation procedure. The activity coefficient results together with the HEm and VEm values have been used to calculate the partial molar excess thermodynamic properties of mixing at infinite dilution. The partial molar excess properties at infinite dilution for decalin mixtures are similar to those for bicyclohexyl mixtures. There is also a similarity between the properties of the tetralin mixtures and the cyclohexylbenzene mixtures. The cycloalkadienes, benzene and the 1-alkynes exhibit a strong dissociation effect on being mixed with the saturated solvents, decalin and bicyclohexyl, but associate strongly with tetralin and with cyclohexylbenzene. The Flory theory bas been used to predict activity coefficients at infinite dilution from the experimentally determined HEm results for { (n-bexane or 1-hexene or 1-hexyne or naheptane or 1-heptene or 1-beptyne) + (a bicyclic compound)}. The theory is much better at predicting values for mixtures where both components are either saturated molecules or are unsaturated molecules than for {saturated + unsaturated} mixtures.
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Akilan, Chandrika. "Thermodynamic and related studies of aqueous copper(II) sulfate solutions." Thesis, Akilan, Chandrika (2008) Thermodynamic and related studies of aqueous copper(II) sulfate solutions. PhD thesis, Murdoch University, 2008. https://researchrepository.murdoch.edu.au/id/eprint/453/.
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This thesis describes a systematic investigation of the thermodynamic quantities associated with the interaction between Cu2+ and SO42- in aqueous solution. A variety of techniques including UV-Visible spectrophotometry, Cu(II) ion-selective electrode potentiometry, dielectric relaxation spectroscopy and titration calorimetry have been used.
The values for the (aq) association constants determined by UV-Vis spectrophotometry in NaClO4 media as a function of ionic strength were in good agreement with published data but were lower than the values obtained from Cu(II) ion -selective electrode potentiometry. The source of this difference was traced to the presence of solvent-separated ion pairs which are only partially detected by UV-Vis spectrophotometry. This was shown by a detailed investigation of CuSO4(aq) over a wide range of concentrations using modern broad-band dielectric relaxation spectroscopy (DRS). This technique revealed the presence of three ion-pair types: double solvent-separated, solvent-shared and contact ion pairs.
Calorimetric titrations using the log KA values determined by potentiometry, have provided for the first time reliable values for the enthalpy and entropy changes associated with complex formation between Cu2+(aq) and SO42-(aq) system over range of ionic strengths (in NaClO4 media). These data were fitted to a specific ion interaction model to obtain the standard state value which was in excellent agreement with the values obtained in other studies and from the DRS work in this study.
In addition, investigations have been carried out into the physicochemical properties, (osmotic coefficients, densities, heat capacities, solubilities and viscosities) of ternary mixtures of CuSO4(aq) with Na2SO4(aq) or MgSO4(aq). The isopiestic measurements (water activities) of the mixtures were in general well described by Zdanovskii's rule, especially for the mixtures of CuSO4 with MgSO4. The densities of the ternary mixtures of CuSO4 with MgSO4 were found to follow Young's rule of mixing but those of CuSO4 with Na2SO4 deviated from linearity. The solubilities of the salts in their ternary mixtures agree well with literature data and show that the solubility of MgSO4 or CuSO4 decreases with increasing Na2SO4 concentration. The viscosities of all the ternary mixtures show clear negative departures from 'Young's rule' type behaviour.
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Akilan, Chandrika. "Thermodynamic and related studies of aqueous copper (II) sulfate solutions /." Akilan, Chandrika (2008) Thermodynamic and related studies of aqueous copper(II) sulfate solutions. PhD thesis, Murdoch University, 2008. http://researchrepository.murdoch.edu.au/453/.
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This thesis describes a systematic investigation of the thermodynamic quantities associated with the interaction between Cu2+ and SO42- in aqueous solution. A variety of techniques including UV-Visible spectrophotometry, Cu(II) ion-selective electrode potentiometry, dielectric relaxation spectroscopy and titration calorimetry have been used.
The values for the (aq) association constants determined by UV-Vis spectrophotometry in NaClO4 media as a function of ionic strength were in good agreement with published data but were lower than the values obtained from Cu(II) ion -selective electrode potentiometry. The source of this difference was traced to the presence of solvent-separated ion pairs which are only partially detected by UV-Vis spectrophotometry. This was shown by a detailed investigation of CuSO4(aq) over a wide range of concentrations using modern broad-band dielectric relaxation spectroscopy (DRS). This technique revealed the presence of three ion-pair types: double solvent-separated, solvent-shared and contact ion pairs.
Calorimetric titrations using the log KA values determined by potentiometry, have provided for the first time reliable values for the enthalpy and entropy changes associated with complex formation between Cu2+(aq) and SO42-(aq) system over range of ionic strengths (in NaClO4 media). These data were fitted to a specific ion interaction model to obtain the standard state value which was in excellent agreement with the values obtained in other studies and from the DRS work in this study.
In addition, investigations have been carried out into the physicochemical properties, (osmotic coefficients, densities, heat capacities, solubilities and viscosities) of ternary mixtures of CuSO4(aq) with Na2SO4(aq) or MgSO4(aq). The isopiestic measurements (water activities) of the mixtures were in general well described by Zdanovskii's rule, especially for the mixtures of CuSO4 with MgSO4. The densities of the ternary mixtures of CuSO4 with MgSO4 were found to follow Young's rule of mixing but those of CuSO4 with Na2SO4 deviated from linearity. The solubilities of the salts in their ternary mixtures agree well with literature data and show that the solubility of MgSO4 or CuSO4 decreases with increasing Na2SO4 concentration. The viscosities of all the ternary mixtures show clear negative departures from 'Young's rule' type behaviour.
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Gao, Yunyi. "Solution Behaviors of Macroions Driven by Non-covalent Interactions." University of Akron / OhioLINK, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=akron1509897811144406.
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Khoee, Bahman. "Soil solution and exchange complex chemistry in a forested watershed." Thesis, McGill University, 1989. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=61821.
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O'Brien, Christine. "Soil solution and streamwater chemistry in a small forested watershed." Thesis, McGill University, 1993. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=68234.
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The relationship between soils, soil water and stream chemistry was investigated for a first order stream in a small forested watershed in the southern Laurentians, Quebec. The study was restricted to near-stream processes, particularly how the chemistry of water leaving a hillslope influenced stream chemistry. For snowmelt, 1986, a number of naturally occurring chemical elements were used to separate stream flow into three subsurface flowpaths: groundwater, solum and upwelling flow. By quantifying upwelling flow, we introduced a new approach to identify solutions forced from the groundwater up through the solum before entering the channel. In upwelling flow, we found that dissolved silicon was reactive and total aluminum, monomeric aluminum, hydronium, magnesium and fluoride were non-reactive. For spring storms, 1992, we used an end member mixing approach to describe streamwater as a combination of chemically distinct solutions from different depths in the soil. Solutions were defined by concentrations of calcium, magnesium, sodium and dissolved silicon. The contributions of water from each soil depth were estimated using the variations in end member chemistry that were measured during the storms. Hydrological reconstructions of the events were possible and it was found that the contribution of water from each depth in podzols is related to the height of the water table in the near-stream soils.
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Saysell, David M. "Aqueous solution chemistry of molybdenum cluster complexes and their derivatives." Thesis, University of Newcastle Upon Tyne, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.295081.
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Seo, Mi-Sook. "Aqueous solution chemistry of heterometallic derivatives containing molybdenum and tungsten." Thesis, University of Newcastle Upon Tyne, 2001. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.364765.
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Wall, Michael D. "Poly(arylsulfone) dendrimers as solution phase supports for combinatorial chemistry." Thesis, University of Warwick, 2002. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.251057.
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Humphrey, K. C. "A dynamic solution of an aspect of wet-end chemistry." Thesis, University of Manchester, 1986. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.292511.
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Jameel, Ambreen. "Molybdenum-phosphate solution chemistry in the preparation of hydrosulphurisation catalysts." Thesis, Manchester Metropolitan University, 1999. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.300354.
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Arumugam, Krishnamoorthy. "Redox chemistry of actinyl complexes in solution : a DFT study." Thesis, University of Manchester, 2012. https://www.research.manchester.ac.uk/portal/en/theses/redox-chemistry-of-actinyl-complexes-in-solution-a-dft-study(ff09f316-847e-498e-a046-1db7bb4c6758).html.
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The chemistry of actinides in solution is a very important aspect of the nuclear fuel cycle, especially as the energy needs of the world continue to increase. However, the radio-active nature of the actinides makes experimentation very difficult and dedicated expensive instruments are required. In addition, the disposal of radio-active waste materials requires a proper understanding of their chemistry at a molecular level. To tackle the problem, and to underpin the experimental studies, in this thesis we have studied the redox chemistry and disproportionation mechanism of actinyl complexes in solution using state-of-the art computational methods. Reduction potentials of actinyl complexes in solution have been estimated in solution using density functional theory (DFT) approaches. Solvation effects were included in the quantum chemistry calculations with the conductor like polarisable continuum model (CPCM) solvation method. First of all, we have validated our computational method by studying a variety of solute cavity definitions within the CPCM solvation model and assessed the performance of a range of DFT functionals to suitable to accurately describe the actinide chemistry in solution. Penta-valent uranyl(V) ions are unstable and readily disproportionate; in this study we have explored outer-sphere electron transfer and disproportionation mechanisms to determine the stability of these ions in solution. We have found that the process of outer-sphere disproportionation is unlikely to occur in non-aqueous solutions, such as DMSO, DMF, DCM, acetonitrile and pyridine, when the uranyl(V) ion is bound with a multi-dentate organic ligand. However, our computational results hypothesise that the presence of a trace of water in the experimental conditions can promote a disproportionation reaction by protonating the uranyl(V) ‘yl’ oxygen atoms and then the electron transfer process would proceed through either inner or outer sphere mechanism. In addition, the effect of alkali metal cations on the outer-sphere disproportionation mechanisms was also studied. Overall it has been shown that DFT can be used to accurately predict the redox properties of actinyl complexes in solution and thus contributing for an effective and efficient design of nuclear material separations, proper as well as safer radioactive waste disposal.
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Näslund, Jan. "Solvated trivalent metal ions in solution : a coordination chemistry study /." Uppsala : Swedish University of Agricultural Sciences, 2000. http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&doc_number=009419319&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA.
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McKay, Kevin J. "The ageing of polyacrylamide in solution." Thesis, University of Huddersfield, 1989. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.293961.
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Knapp, Caroline Mary. "Solution reactivity studies of group 15 Zintl ions." Thesis, University of Oxford, 2013. http://ora.ox.ac.uk/objects/uuid:0196fc28-2915-45f4-878d-12a6a1f01129.
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The reactivity of group 15 Zintl ions, E73– (E = P, As), towards a number of transition and post-transition metal reagents has been studied. The synthesis and characterisation of the resulting novel cluster anions are described herein. The reactions of E73– with [Cu5(mes)5], MPh2 (M = Zn, Cd) and InPh3 yielded the Cu–Cu bridged species [Cu2(E7)2]4– (E = P, As), the group 12 bridged cluster anions [M(E7)2]4– (M = Zn: E = P, As; M= Cd: E = P), and the In-functionalised Zintl ions [E7InPh2]2–, respectively. P73– and As73– have been found to react with a number of metal salts, namely [M(nbe)3][SbF6] and MCl (M = Ag, Au), InCl3, TlCl and MI2 (M = Sn, Pb). These reactions formed the Ag–Ag and Au–Au bridged complexes [M2(HP7)2]2– (M = Ag, Au), the In-bridged species [In(E7)2]3– (E = P, As), the Tl-derivatised Zintl ions [TlE7]2– (E = P, As), and the sixteen vertex cluster anions [ME15]3– (M = Sn, Pb; E = P, As). The reactivity of P73– towards a series of group 8 compounds has also been studied. The reactions of P73– with FeCl2 and [Ru(PPh3)3Cl2] produced [M(HP7)2]2- (M = Fe, Ru). NMR studies showed that these species can be deprotonated to form [M(P7)2]4– (M = Fe, Ru). These Fe and Ru complexes are isoelectronic with ferrocene. In addition, P73– reacts with [Ru(COD)(η3-CH2C(CH3)CH2)2] to form [(C4H7)P7Ru(COD)]2–. Both P73– and As73– undergo transition metal mediated activation reactions in the presence of [Co(PEt2Ph2)(mes)2], yielding [Co(η5-P5){η2-HP2(mes)}]2– and [Co([η3-As3){η4-As4(mes)2}]2–, respectively.
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Miletti, Teresa. "Enzyme flexibility studied by solution NMR spectroscopy." Thesis, McGill University, 2013. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=119414.
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The important connection between dynamics, structure and function of enzymes still remains unclear and is, hence, an interesting relationship to investigate. In this thesis, the enzymes NADH oxidase (NOX) from Thermus thermophilus and mycobacterium tuberculosis (Mtb) protein tyrosine phosphatase B (PtpB) were chosen as systems to study the influence of solution conditions on protein structure and flexibility in relation to their catalytic activity. Nuclear magnetic resonance (NMR) and isothermal titration calorimetry (ITC) techniques were used in the study of NOX. NMR and differential scanning fluorimetry (DSF) were utilized to assess the sample stability of PtpB under various buffer conditions.NOX is a 54 kDa homodimeric enzyme with many potential biotechnology applications. It accepts cofactors flavin mononucleotide (FMN) or flavin adenine dinucleotide (FAD). It has high thermal stability and its activity increases with the addition of low concentrations of urea. Using enzymes in vitro provides us a lot of freedom to control its environment, which is useful to look at changes occurring under different conditions. Thus, NMR allowed us to investigate these interesting characteristics on NOX dynamics and structure. When Mtb infects host cells it secrets among others, PtpB, to disrupt signalling pathways and blunts immune responses. PtpB contains a two-helix lid that completely buries the active site and it is proposed that it has evolved as a novel mean of protection against host chemical defences and affords substrate access. An investigation of conformational dynamics of the lid domain of PtpB using NMR would elucidate a relation between conformation and function of Ptpb, which to date, is still unknown and would contribute to the development of inhibitors as potential drugs. In order to do this, it is essential to obtain a stable sample that will give optimal quality NMR spectra. NMR and DSF were used to optimize PtpB NMR sample conditions and spectral quality. We employed a suite of novel 15N NMR relaxation experiments to estimate the extent of broadening due to microsecond-timescale motions and to measure exchange-free transverse relaxation rates on a per-residue basis of NOX. These measurements allowed us to identify several residues involved in dynamical processes. Moreover, order parameters, S2, determined from standard 15N T1, T2 and {1H}-15N steady NOE experiments, allowed the identification of additional residues characterized by motions on nanosecond-picosecond time scales. We then investigated the effects of temperature, urea addition, cofactor and NAD+ product binding to NOX using NMR and ITC. For each condition studied, chemical shift displacement of NMR peaks is significant relative to all other peaks only for a reoccurring small subset of residues. This cluster of residues is located around the active site of the enzyme and thus, suggests evidence of a relationship between concerted conformational rearrangement of NOX structure and NOX catalytic activity. An increase in NMR spectral quality and a NMR sample of PtpB with increased thermal stability, higher yields and reduced aggregation was obtained for further NMR dynamic experiments. This was achieved by optimizing the sample conditions by performing several NMR titrations and DSF experiments. Assessing the thermal stability of enzymes with different additives using DSF could be easily introduced during the elaboration of protein purification protocols as a routine method to optimize NMR sample conditions for NMR studies.Le lien important entre la dynamique, la structure et la fonction des enzymes n'est pas encore bien défini et est donc une relation intéressante à étudier. Dans cette thèse, les enzymes NADH oxydase (NOX) de Thermus thermophilus et mycobacterium tuberculosis protéine tyrosine phosphatase B (PtpB) sont les systèmes choisis pour étudier l'influence des conditions de solution sur la structure et la flexibilité des protéines par rapport à leur activité catalytique. Les techniques de résonance magnétique nucléaire (RMN) et de calorimétrie de titration isothermique (ITC) ont été utilisées dans l'étude de NOX. La RMN et la fluorimétrie différentielle à balayage (DSF) ont été utilisées pour évaluer la stabilité de l'échantillon de PtpB dans diverses conditions de tampons. NOX est une enzyme homodimérique avec de nombreuses applications biotechnologiques potentielles. NOX accepte les cofacteurs flavine mononucléotide (FMN) ou flavine adénine dinucléotide (FAD). L'enzyme a une stabilité thermique élevée et son activité augmente avec l'addition de faibles concentrations d'urée. Utiliser des enzymes in vitro donne beaucoup de liberté pour contrôler leur environnement, utile pour examiner les changements qui se produisent dans différentes conditions. Ainsi, RMN nous a permis d'étudier ces caractéristiques intéressantes sur la dynamique et la structure de NOX. Lorsque Mtb infecte les cellules, il secrète PtpB qui perturbe les voies de signalisation et affaibli les réponses immunitaires. PtpB contient un couvercle de deux hélices qui enterre complètement le site actif et il est proposé qu'il ait évolué ainsi en protection contre les défenses chimiques et permet un accès au substrat. Une étude de la dynamique du domaine du couvercle de PtpB utilisant la RMN éluciderait la relation entre la conformation et la fonction de PTPB et contribuerait au développement d'inhibiteurs en tant que médicaments potentiels. Pour ceci, il est essentiel d'obtenir un échantillon stable qui donnera des spectres RMN de qualité optimale. RMN et DSF ont été utilisés pour optimiser les conditions d'échantillonnage de PtpB pour la RMN et la qualité spectrale. Nous avons utilisé une suite de nouvelles expériences de relaxation de 15N par RMN pour estimer l'ampleur de l'élargissement des signaux en raison de mouvements à l'échelle de temps des microsecondes et de mesurer les taux de relaxation transversale sans échange pour chaque résidu de NOX. Ces mesures nous ont permis d'identifier plusieurs résidus impliqués dans les processus dynamiques. De plus, les paramètres d'ordre, S2, déterminées à partir des expériences standards de T1, T2 et NOE, ont permis d'identifier des résidus additionnels caractérisés par des mouvements sur des échelles de temps de nanosecondes à picosecondes. Nous avons ensuite étudié les effets de la température, urée, la liaison de cofacteur et du produit à NOX en utilisant la RMN et le ITC. Pour chaque condition étudiée, la variation de déplacement chimique des signaux RMN n'est significative par rapport à tous les autres signaux que pour un petit sous-ensemble récurrent de résidus. Cet amas de résidus est situé autour du site actif de l'enzyme et ainsi, suggère preuve d'une relation entre un réarrangement conformationnel concertée de la structure de NOX et de son activité catalytique. Une augmentation de la qualité spectrale de RMN et un échantillon de PtpB pour la RMN avec une meilleure stabilité thermique, des rendements plus élevés et une agrégation réduite ont été obtenus pour de futures expériences dynamiques par RMN. Ceci a été réalisé en optimisant les conditions de l'échantillon en effectuant plusieurs titrages par RMN et des expériences de DSF. L'évaluation de la stabilité thermique des enzymes avec différents additifs à l'aide de DSF pourrait facilement être introduit lors de l'élaboration de protocoles de purification de protéines comme une méthode routinière pour optimiser les conditions d'échantillons pour les études par RMN.
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Nguyen, Can Phvoc 1972. "Solution and solid-phase synthesis of sialooligomers." Thesis, The University of Arizona, 1998. http://hdl.handle.net/10150/291822.
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The solution phase synthesis of amide-linked derivatives of sialic acid has been achieved. The N-acetyl group on sialic acid was removed via N-BOC protection of the lactam and ensuing displacement with NaOMe. Subsequent removal of the BOC protecting group group with TFA resulted in the free amine which was then coupled with the free acid using BOP, Hunig's base, and NMP. These compounds may afford greater solubility than previously synthesized amide-linked carbohydrate amino acids and may give rise to novel helical structures. The efficacy of using monomer units of sialic acid in solid-phase oligomer synthesis has also been studied. The peracetylated FMOC-protected derivative of sialic acid which has been shown to be amenable to solid-phase synthesis has also been synthesized. However, difficulties were encountered during the solid-phase synthesis of these sialooligomers due to transacetylation of the acetate groups to re-form the N-acetyl bond.
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Brewer, Scott Harmon. "Solution and Surface Characterization of DNA and Proteins." NCSU, 2004. http://www.lib.ncsu.edu/theses/available/etd-11292004-160406/.
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A variety of experimental spectroscopic techniques complemented by theoretical calculations when appropriate were used to investigate DNA adlayers on surfaces and proteins in solution. The formation and characterization of DNA adlayers on gold and indium tin oxide surfaces were characterized along with subsequent surface DNA hybridization. Prior to the modification of indium tin oxide surfaces with DNA, the optical and electronic properties of this metal oxide, fluorine doped tin oxide and iridium oxide were investigated. The detection of DNA hybridization on indium tin oxide surfaces utilized gold nanoparticle labeled target ssDNA. Further work on gold surfaces was performed using infrared spectroscopy to detect sugar binding to a phenylboronic acid terminated self-assembled monolayer. The binding properties and stability of gold nanoparticles were investigated by characterizing citrate and bovine serum albumin binding to gold surfaces and the stability of particles stabilized by these molecules. The stability and folding kinetics of the three helix bundle protein, villin headpiece subdomain was also investigated in addition to a theoretical investigation of the vibrational Stark effect. Finally, a time resolved step scan FTIR spectrometer was implemented with five microsecond time resolution.
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ZHOU, YIFAN. "SELF-ASSEMBLY AND SELF-RECOGNITION BEHAVIORS OF AMPHIPHILIC MACROMOLECULES IN SOLUTION." University of Akron / OhioLINK, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=akron1619093496152417.
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Demers, Audrey Gertrude. "Structural studies of glycoproteins in solution." Case Western Reserve University School of Graduate Studies / OhioLINK, 1990. http://rave.ohiolink.edu/etdc/view?acc_num=case1054759177.
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Ploetz, Elizabeth Anne. "Fluctuation solution theory." Diss., Kansas State University, 2014. http://hdl.handle.net/2097/18390.
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Doctor of PhilosophyDepartment of Chemistry
Paul E. Smith
The Kirkwood-Buff (KB) theory of solutions, published in 1951, established a route from integrals over radial (pair) distribution functions (RDFs) in the grand canonical ensemble to a set of thermodynamic quantities in an equivalent closed ensemble. These “KB integrals” (KBIs) can also be expressed in terms of the particle-particle (i.e., concentration or density) fluctuations within grand canonical ensemble regions. Contributions by Ben-Naim in 1977 provided the means to obtain the KBIs if one already knew the set of thermodynamic quantities for the mixture of interest; that is, he provided the inversion procedure. Thus, KB theory provides a two-way bridge between local (microscopic) and global (bulk/thermodynamic) properties. Due to its lack of approximations, its wide ranging applicability, and the absence of a competitive theory for rigorously understanding liquid mixtures, it has been used to understand solution microheterogeneity, solute solubility, cosolvent effects on biomolecules, preferential solvation, etc. Here, after using KB theory to test the accuracy of pair potentials, we present and illustrate two extensions of the theory, resulting in a general Fluctuation Solution Theory (FST). First, we generalize KB theory to include two-way relationships between the grand canonical ensemble’s particle-energy and energy-energy fluctuations and additional thermodynamic quantities. This extension allows for non-isothermal conditions to be considered, unlike traditional KB theory. We illustrate these new relationships using analyses of experimental data and molecular dynamics (MD) simulations for pure liquids and binary mixtures. Furthermore, we use it to obtain conformation-specific infinitely dilute partial molar volumes and compressibilities for proteins (other properties will follow) from MD simulations and compare the method to a non-FST method for obtaining the same properties. The second extension of KB theory involves moving beyond doublet particle fluctuations to additionally consider triplet and quadruplet particle fluctuations, which are related to derivatives of the thermodynamic properties involved in regular KB theory. We present these higher order fluctuations obtained from experiment and simulation for pure liquids and binary mixtures. Using the newfound experimental third and fourth cumulants of the distribution of particles in solution, which can be extracted from bulk thermodynamic data using this extension, we also probe particle distributions’ non-Gaussian nature.
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Li, Hui. "UNDERSTANDING AND CONTROLLING THE INTERMOLECULAR INTERACTION BETWEEN MACROIONS IN DILUTE SOLUTION." University of Akron / OhioLINK, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=akron1548322091331009.
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Tromans, Andrew J. "Solution chemistry of some dicarboxylate salts of relevance to the Bayer process /." Access via Murdoch University Digital Theses Project, 2003. http://wwwlib.murdoch.edu.au/adt/browse/view/adt-MU20040730.140604.
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Haward, Mark T. "Spectroscopy and photochemistry in liquid xenon solution." Thesis, University of Nottingham, 1991. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.334777.
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Alexander, P. H. V. "Solution-membrane interactions by non-ionic surfactants." Thesis, Cardiff University, 1985. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.304749.
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Webster, Lee. "Polyelectrolyte complex formation in dilute aqueous solution." Thesis, University of Salford, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.360472.
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Ibison, Paul. "Oscillations and instabilities in solution phase reactions." Thesis, University of Leeds, 1991. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.305437.
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