Abstract: Aqueous solutions of 2,2,2-trifluoroethanol appears to show a structural transition at alcohol mole fraction equal to x<sub>TFE</sub>= 0.05, that can be concluded from a discontinuity of the speed of sound. At the same concentration, a discontinuity was observed in the parameters of the long-living component of the positron annihilation spectrum. Moreover, the partial molar volumes of components show transition-like behaviour in the range of low solute contents, which is significantly different from non-substituted ethanol. The peculiarities of the low concentration system correlate with minor infrared spectra changes assigned to mode composed of the CH<sub>2</sub> bending and CF<sub>3</sub> stretching internal vibrations being sensitive to polarity of the hydration shell surrounding the solute. Majority of the spectral changes arises from a gradual shift of the equilibrium between transâgauche isomers when the composition of solution is changing. A possible explanation for the peculiar behavior of the system is a thermodynamic equilibrium between hydrated monomers and dimers at that respective mole number.
Notes: CAS Section: Phase Equilibriums, Chemical Equilibriums, and Solutions
Abstract: Additive manufacturing techniques can be used to produce micro-porous structures with global morphological properties that are highly controlled through robust computer design. Despite these advantages, most of these techniques still hold several functional constraints, resulting from present technical device limits and consequently the inability to control surface morphology at a microscale level. In this study, a novel protocol for surface modification of 3D titanium alloy-based open porous structures is developed, which applies a combination of chemical etching (CHE) and electrochemical polishing (ECP) using HF-based solutions. This protocol achieves significant and controllable roughness reduction of additive manufactured 3D Ti6Al4V open porous structures. Chemical etching mainly removes the attached powder grains, while ECP further decreases the roughness. In this way the heterogeneity of the strut surface roughness throughout the full 3D structure is effectively removed.
Abstract: A model assuming that equilibrium reaction of formation of non-compressible dimers dominates in and governs the acoustic properties of liquid mixtures of alcohols in inert hydrocarbon solvents was developed. It was found to describe satisfactorily the observed compressibility dependences on composition of the title systems, in particular those containing long-chained components. This attempt allows to estimate the dimerization equilibrium constants from the compressibility data.
Abstract: The parabolic-like plots of compressibility vs. concentration of non-electrolytes (ethanol as the example) in water are explained and described assuming the hydrate formation equilibrium reaction. Only two fitted parameters, the hydration number n<sub>h</sub> and the cumulative formation constant of the hydrate β<sub>n<sub>h</sub></sub> are able to reproduce the experimental data, including the minima of κ<sub>S</sub> vs. composition at low solute contents. Another discussed option is a set of subsequent equilibrium reactions of hydration from which formation constants can also be determined. Calculations were performed for water-ethanol system, and the results were compared with those obtained by the model developed by us recently.
Notes: Special Workshop Issue: Selected Papers Presented at the 15<sup>th</sup> Workshop on Photoacoustics and Thermal Wave Methods and the 6<sup>th</sup> Workshop on Molecular Acoustics, Relaxation and Calorimetric Methods
Abstract: Car-Parrinello Molecular Dynamics and acoustic method have been applied to determine the hydration of HCO<sub>3</sub><sup>-</sup> and CO<sub>3</sub><sup>2-</sup> ions in aqueous solution. From CPMD simulations the hydration numbers are 5.3 and 8.5 for the HCO<sub>3</sub><sup>-</sup> and CO<sub>3</sub><sup>2-</sup> ions, respectively. From speed of sound and density measurements the hydration numbers for HCO<sub>3</sub><sup>-</sup> and CO<sub>3</sub><sup>2-</sup> are 5.5 and 10.2, respectively. Our attempt to answer the old question concerning the status of HCO<sub>3</sub><sup>-</sup> in solution quite well support the earlier spectroscopic results that no (HCO<sub>3</sub><sup>-</sup>)<sub>2</sub> is present in the solution but the existence of the minor amount of dimers cannot be definitely excluded.
Abstract: Untypical changes of molar volume and compressibility of liquid water with temperature are analyzed using a very simple model assuming that a temperature-dependent equilibrium exists between two states of water molecules in liquid. The fittings show, independent on extremely rough assumptions and simplifications applied, that the two-state model of liquid water is still able to reproduce the molar volumes almost perfectly but in the case of compressibility physically nonrealistic results are obtained. These results generate questions and reservations about opportunity of determining the number of states describing liquid water.
Abstract: In this paper the parabolic-shaped dependences of compressibility κ<sub>S</sub> of a non-electrolyte in water solvent on concentration are explained and described semi-quantitatively in terms of hydrate formation equilibrium reaction. It was demonstrated that only two fitted parameters, the hydration number n<sub>h</sub> and the formation constant of the hydrate K are sufficient to reproduce satisfactorily the experimental data, in particular the characteristic minimums of κ<sub>S</sub> vs. composition, observed at low contents of solutes.
Abstract: In this paper the results of compressibility of aqueous solutions of amino acids in water and in aqueous HCl and NaOH solutions at 25 °C are presented. The effect of the charged protonated amino groups and deprotonated carboxylic groups on the hydration number was tested. The idea of additivity of the hydration number with the constituents of the solute molecule was successfully applied and discussed.
Abstract: In the present article the applicability of the Pasynski method of determination of hydration numbers of simple organic compounds in aqueous solvents of fixed pH at 25 °C from speed-of-sound and density measurements is tested and discussed. It was shown that for solutes which do not undergo protolytic reactions with a solvent the resulting values of hydration numbers are independent on the system pHâfor these solutes n<sub>h</sub> can be determined both in pure aqueous solutions and in mixtures containing ions. For solutes which undergo reactions with an acid or base, the Pasynski method yields hydration numbers which are a combination of compressibilities of substrates and products of occurring reactions.
Notes: Special Workshop Issue: Selected Papers Presented at the 14<sup>th</sup> Workshop on Photoacoustics and Thermal Wave Methods and the 5<sup>th</sup> Workshop on Molecular Acoustics, Relaxation and Calorimetric Methods. In Honor of Prof. Stefan Ernst (75<sup>th</sup> Birthday)
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<li>Shashi Kant, Dharmvir Singh, Sunil Kumar, Molar volume and ultrasonic studies of some alkaline earth metal chlorides in water + NaCl + fructose system, <i>Archives of Applied Science Research</i> <b>3</b> (2011) 70-84
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<li>Shashi Kant, Sunil Kumar, Manish Kumar, Vikas Bharti, Acoustic studies of hydrated nickel sulphate in aqueous ascorbic acid systems, <i>Der Chemica Sinica</i> <b>3</b> (2012) 166-174
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Abstract: Positron annihilation measurements were performed in aqueous solutions of β-cyclodextrin, as well as in solid mixtures of this sugar with a long-chained alcohol, n-nonanol. Additionally, acoustic (sound speed, density and
compressibility) experiments were done in aqueous β-cyclodextrin and tert-butanol systems and in a three-component water-β-cyclodextrin-tert-butanol system. The results show that in aqueous solution cyclodextrin does not form inclusive complexes with alcohol, while solid sugar-alcohol mixtures undergo slow changes in time, most probably caused by exchange of guest between interior and exterior of the host molecule.
Notes: Proceedings of the 38<sup>th</sup> Polish Seminar on Positron Annihilation (PSPA'09)
8-12 June 2009, Kazimierz Dolny, Poland
Abstract: In this letter the results of compressibility measurements made on 1:1 electrolytes containing normal aliphatic chains (monoalkylammonium salts and those of normal aliphatic acids) in water and aqueous HCl and NaOH solutions at 25ºC have been used to calculate the hydration numbers of ions. It was shown that they depend mainly on the ionic size. The idea of additivity of the hydration number n<sub>h</sub> with the constituents of solute molecule was successfully applied. The contributions from âNH<sub>3</sub><sup>+</sup> and âCOO<sup>â</sup> groups to the total n<sub>h</sub> of salts were determined.
Abstract: The method of Passynski of calculating the solvation numbers from compressibility was applied to solutions of short-chained normal alcohols in n-heptane and n-propanol. The dependences of solvation numbers on length of the solute molecules are surprisingly similar for both solvents. Applicability of the acoustic method for determining the solvation numbers in nonaquous systems, as well as for investigation of intermolecular interactions in them was proved. Some structural similarity of associated alcohol and hydrocarbon in liquid state is suggested.
Notes: Optical and Acoustical Methods in Science and Technology
Abstract: The acoustic method of Pasynski was applied to investigate solvation of short-chained normal alcohols in n-heptane and n-propanol as solvents. For both solvents, the dependence of solvation numbers on length of the solute molecules is surprisingly similar, except that for the shortest alcohols. Applicability of the acoustic method for investigation of intermolecular interactions in non-aqueous liquid systems was proved. Hypothesis on some structural similarity of associated alcohol and hydrocarbon in liquid state is formulated.
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<li>Marzena Dzida, Leokadia Waleczek, Speed of sound, density, and heat capacity for (2-methyl-2-butanol + heptane) at pressures up to 100 MPa and temperatures from (293 to 318) K. Experimental results and theoretical investigations, <i>Journal of the Chemical Thermodynamics</i> <b>42</b> (2010) 312-322
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Abstract: Sound velocity and density were measured at 298.15âK in a number of very diluted aqueous solutions of simple non-electrolytes: alcohols, amines and acids. From these data the adiabatic compressibilities were calculated, and further the hydration numbers of solutes using the Passynski formula. It was found that all the homologous series under investigation exhibit linear concentration dependence of compressibility â and, consequently, that of the hydration numbers â up to concentrations of ca. 0.01 mole fraction or more. The slopes of these dependences are decreasing and n<sub>h</sub>'s are increasing with the molecular mass of the solute. This observation suggests that hydration numbers n<sub>h</sub> are additive with the constituents of the molecule. Moreover, it would also imply the conclusion that local loss in compressibility of water solvent caused by hydration is very short in distance. To test the above assumption the hydration numbers were calculated using partial hydration numbers (i.e. those assigned to specific functional groups of the solute molecules), the latter are fitted parameters. The obtained values of partial n<sub>h</sub>'s are ca. 0.5 for âOH group, ca. 1.15 for âCOOH and âNH<sub>2</sub> and from 0.5 to ca. 1.3 for hydrocarbon elements of the hydrophobic chain (âCH<sub>2</sub>â and âCH<sub>3</sub> groups). The obtained total n<sub>h</sub>'s are surprisingly close to the experimentally obtained hydration numbers. There are, however, systems where differences between calculated and experimental n<sub>h</sub>'s are exceeding the experimental uncertainty; they are amino acids and diols, particularly α,Ï-diols. The reasons are, most possibly, interaction of the hydration shells of the hydroxyl groups in the latter case and formation of two charged sites in the zwitterionic form of the former ones.
Notes: Wave and Quantum Acoustics
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<li>Roger Y. Tam, Sandra S. Ferreira, Pawel Czechura, Jennifer L. Chaytor, Robert N. Ben, Hydration index â A better parameter for explaining small molecule hydration in inhibition of ice recrystallization, <i>Journal of the American Chemical Society</i> <b>130</b> (2008) 17494-17501
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<li>Kamila KieÅek, Wojciech Marczak, Hydration of non-electrolytes in H<sub>2</sub>O and D<sub>2</sub>O investigated by Passynskiâs method, <i>International Journal of Thermophysics</i> <b>31</b> (2010) 77-84
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<li>Ayelet Shvalb, Yitzhak Mastai, Meir Shinitzky, Chiral configuration of the hydration layers of D- and L-alanine in water implied from dilution calorimetry, <i>Chirality</i> <b>22</b> (2010) 587-592
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<li>Katja Arand, David Stock, Markus Burghardt, Markus Riederer, pH-dependent permeation of amino acids through isolated ivy cuticles is affected by cuticular water sorption and hydration shell size of the solute, <i>Journal of Experimental Botany</i> <b>61</b> (2010) 3865-3873
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<li>Robert N. Ben, Roger Tam, PaweÅ Czechura, Antifreeze glycoprotein analogues and uses thereof, <i>United States Patent Application</i> 20100068692 A1
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<li>Roger Tam, Studies into the structural features of C-linked antifreeze glycoprotein analogues responsible for ice-recrystallization inhibition activity, <i>Doctoral Thesis, Ottawa-Carleton Chemistry Institute, Faculty of Graduate & Postdoctoral Studies University of Ottawa, </i> Ottawa, Canada, 2011
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Abstract: It was shown for dilute aqueous solutions of few homologous series of organic non-electrolytes that the effect of solutes on compressibility decrease is directly linked to the length of their molecules and the groups, which are their constituents.
The contributions of the groups â constituents of solute molecules â have been determined and discussed. It seems possible now to predict compressibility of aqueous solutions of organic non-electrolytes only from their structural formulae.
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<li>Laura-Marinela Ailioaie, Elena Filip, Dana-Ortansa Dorohoi, Intermolecular interactions in water-ethanol mixtures, studied by ultrasound technique, <i>Revista De Chimie</i> <b>59</b> (2008) 734-738
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<li>Thomas Schöck, Thomas Becker, Sensor array for the combined analysis of waterâsugarâethanol mixtures in yeast fermentations by ultrasound, <i>Food Control</i> <b>21</b> (2010) 362-369
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<li>Kamila KieÅek, Wojciech Marczak, Hydration of non-electrolytes in H<sub>2</sub>O and D<sub>2</sub>O investigated by Passynskiâs method, <i>International Journal of Thermophysics</i> <b>31</b> (2010) 77-84
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<li>Thomas Schöck, Mohamed Hussein, Thomas Becker, Konzentrationsbestimmung in Wasser-Zucker-Ethanol-Gemischen mittels adiabatischer Kompressibilität und Dichte (Concentration determination in water-sugar-ethanol-mixtures via adiabatic compressibility and density), <i>TM-Technisches Messen</i> <b>77</b> (2010) 30-37
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Abstract: In this communication, we report the compressibility measurements made on amino acids in water at 25<sup>o</sup>C, compared with aqueous short-chained amines and carboxylic acids. The effect of the charge caused by protonation of the amino group and/or deprotonation of the carboxylic one was tested. The concept of additivity of the hydration number with the constituents of solute molecule was applied and discussed.
Notes: Optical and Acoustical Methods in Science and Technology
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<li>Katja Arand, David Stock, Markus Burghardt, Markus Riederer, pH-dependent permeation of amino acids through isolated ivy cuticles is affected by cuticular water sorption and hydration shell size of the solute, <i>Journal of Experimental Botany</i> <b>61</b> (2010) 3865-3873
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<li>Katja Arand, Charakterisierung hydrophiler Permeationswege in der pflanzlichen Kutikula anhand der Permeationseigenschaften ionischer Aminosäuren, <i>Dissertation zur Erlangung des naturwissenschaftlichen Doktorgrades der Julius-Maximilians-Universität Würzburg</i>, Würzburg, 2010
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Abstract: The positron annihilation and acoustic methods were applied to investigate solvation of potassium iodide, and tetra-n-butylammonium iodide in methanol. The acoustic results show that the influence of KI on the structure of liquid is stronger but shorter in their range than that of (C<sub>4</sub>H<sub>9</sub>)<sub>4</sub>NI, although the solvation numbers are lower for KI. The solvation numbers of ions (five for K<sup>+</sup>, seven for (C<sub>4</sub>H<sub>9</sub>)<sub>4</sub>N<sup>+</sup> and two for I<sup>â</sup>) are deduced.
The positron annihilation suggests that the effect of KI on liquid methanol structure is stronger but shorter in range, leading to formation of small but more compressed solvates.
Abstract: Applicability of the acoustic Pasynski method of determination of hydration numbers for non-electrolytic aqueous solutions has been tested and discussed. It was shown for dilute aqueous solutions of few homologous series of organic non-electrolytes that the hydration numbers are strongly and directly depending on the length of solute molecules and the groups which are their constituents. Thus, the results suggest that hydration is an additive parameter, although its mechanisms are different.
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<li>Mohammed Taghi Zafarani-Moattar, Somayeh Emamian, Sholeh Hamzehzadeh, Effect of temperature on the phase equilibrium of the aqueous two-phase poly(propylene glycol) + tripotassium citrate system, <i>Journal o Chemical and Engineering Data</i> <b>53</b> (2008) 456-461
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<li>Kamila KieÅek, Wojciech Marczak, Hydration of non-electrolytes in H<sub>2</sub>O and D<sub>2</sub>O investigated by Passynskiâs method, <i>International Journal of Thermophysics</i> <b>31</b> (2010) 77-84
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<li>Marco Cespi, Giulia Bonacucina, Giovanna Mencarelli, Stefania Pucciarelli, Gianfabio Giorgioni, Giovanni F. Palmieri, Monitoring the aggregation behaviour of self-assembling polymers through high-resolution ultrasonic spectroscopy, <i>International Journal of Pharmaceutics</i> <b>388</b> (2010) 274-279
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<li>Ð. Ð. Смолин, Ð. Ð. ÐодловÑенко, ÐлиÑние Ð´Ð»Ð¸Ð½Ñ ÑглеводоÑодной Ñепи ноÑмалÑнÑÑ Ð°Ð»Ð¸ÑаÑиÑеÑÐºÐ¸Ñ ÑпиÑÑов на Ð¸Ñ Ð²Ð·Ð°Ð¸Ð¼Ð¾Ð´ÐµÐ¹ÑÑвие Ñ Ð°Ð´ÑоÑбиÑованнÑм киÑлоÑодом на поликÑиÑÑаллиÑеÑком плаÑиновом ÑлекÑÑоде, <i>ÐлекÑÑоÑимиÑ</i> <b>46</b> (2010) 387-394
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<li>A.V. Smolin, B.I. Podlovchenko, The effect of hydrocarbon chain length in normal aliphatic alcohols on their reaction with oxygen adsorbed on polycrystalline platinum electrode, <i>Russian Journal of Electrochemistry</i> <b>46</b> (2010) 367-373
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<li>Katja Arand, David Stock, Markus Burghardt, Markus Riederer, pH-dependent permeation of amino acids through isolated ivy cuticles is affected by cuticular water sorption and hydration shell size of the solute, <i>Journal of Experimental Botany</i> <b>61</b> (2010) 3865-3873
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<li>Katja Arand, Charakterisierung hydrophiler Permeationswege in der pflanzlichen Kutikula anhand der Permeationseigenschaften ionischer Aminosäuren, <i>Dissertation zur Erlangung des naturwissenschaftlichen Doktorgrades der Julius-Maximilians-Universität Würzburg</i>, Würzburg, Germany, 2010
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<li>Zhuo Zhang, Solvent effects on the molecular structures of crude gliadins as revealed by density and ultrasound velocity measurements, <i>Master Thesis, Department of Food Science, University of Manitoba</i>, Winnipeg, Canada, 2010
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<li>Marco Cespi, Giulia Bonacucina, Giovanna Mencarelli, Gianfabio Giorgioni, Giovanni Filippo Palmieri, Evaluation of polymer mucoadhesiveness by the use of acoustic spectroscopy, <i>AAPS PharmSciTech</i> <b>11</b> (2010) 1232-1236
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<li>Tejwant Singh, Arvind Kumar, Thermodynamics of dilute aqueous solutions of imidazolium based ionic liquids, <i>The Journal of Chemical Thermodynamics</i> <b>43</b> (2011) 958-965
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<li>Annalisa Boscaino, Kevin J. Naidoo, The extent of conformational rigidity determines hydration in nonaromatic hexacyclic systems, <i>The Journal of Physical Chemistry B</i> <b>115</b> (2011) 2608-2616
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<li>Rita Mehra, Brij Bihari Malav, Acoustic, volumetric and viscometric studies of DL-alanine in aqueous galactose solution in the presence of sodium chloride at 298, 308 and 318 K, <i>Research Journal of Pharmaceutical, Biological and Chemical Sciences</i> <b>2</b> (2011) 709-719
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<li>Rita Mehra, Brij Bihari Malav, Molecular interaction study of glycine in aqueous galactose solution and effect of sodium chloride at 298 to 318âK, <i>Physics and Chemistry of Liquids: An International Journal </i> <b>50</b> (2012) xxx-xxx DOI:10.1080/00319104.2011.604778
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Abstract: The results of optical spectroscopic (UV-Vis, absorption, and emission), acoustic (sound velocity of precursor solutions, the solvation numbers of ions in these solutions), and positron annihilation of glasses are presented and discussed for silica glasses obtained by the alcoholic sol-gel technique, doped with selected lanthanides and with some addition of ethylene glycol. The aim of these investigations was the determination of the local structure of glass close to lanthanide ions and its influence on the optical properties of the material. The results show that the existence of alcohol-glycol solvates in glasses decrease the number of empty voids in its structure as well as the size of the remaining ones. One can suppose that this is caused by cooperative interactions of glycol molecules with the network of hydrogen bonds of the glass.
Notes: Proceedings of the 36<sup>th</sup> Polish Seminar on Positron Annihilation, Turawa, Poland, 2006
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<li>Janina Legendziewicz, MaÅgorzata Guzik, Jacek GliÅski, Kazimierz Jerie, Andrzej Baranowski, Andrzej Kochel, Application of spectroscopy and positron annihilation methods in studies of the gel-glasses materials, <i>Journal of Alloys and Compounds</i> <b>451</b> (2008) 172-178
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Abstract: We report the results of acoustic and positron annihilation measurements in aqueous solutions of acetonitrile (CH<sub>3</sub>CN). Hydrophobicity of the solute is discussed, as well as the possibility of describing the title system in terms of hydrophobic solvation. The concept of Levay et al. of calculating the "ideal" positronium lifetimes is applied, basing on the mean volume of cavities (holes) in liquid structure available for positronium pseudoatom. The same calculations performed using the Tao model of annihilation yield very different results. It can be concluded that either acetonitrile forms with water clathrate-like hydrates of untypical architecture, or it is too weak hydrophobic agent to form clathrate-like hydrates at all. The former interpretation seems to be more probable.
Abstract: A new attempt in acoustical investigations of interactions between components of liquid solution is presented and tested. It was shown, basing on very simple assumptions and relatively simple experiment, that changes in the concentration dependences of the adiabatic compressibility (calculated from sound velocity and density data) are influenced by intermolecular interactions occurring in solutions. However, it was also shown that these changes are not very strong and the strongest are caused by processes, where the total number of ions and/or their charge density are changing. We also suggest that for some weak association-like processes the compressibility can remain almost undisturbed and, consequently, not sensitive for them.
Notes: 34<sup>th</sup> Winter School on Wave and Quantum Acoustics, Ustron, Poland, 28 February - 4 March 2005
Abstract: We report the results of acoustic and positron annihilation measurements in aqueous solutions of acetonitrile (CH<sub>3</sub>CN). Hydrophobicity of the solute is discussed, as well as the possibility of describing the title system in terms of hydrophobic solvation. A new method of calculating the ââidealââ positronium lifetimes is proposed, based on the mean volume of cavities (holes) in liquid structure available for positronium pseudoatom. The results are almost identical with those obtained from molar volumes using the concept of Levay et al. On the other hand, the same calculations performed using the ââbubbleââ model of annihilation yield very different results. It seems that either acetonitrile forms with water clathrate-like hydrates of untypical architecture, or it is too weak hydrophobic agent to form clathrate-like hydrates at all. The former interpretation seems to be more probable.
Abstract: In this work speeds of sound and the densities of diluted aqueous solutions of a few homologous series of alcohols, glycols, polyhydroxylic alcohols, ketones, mono- and dicarboxylic acids, amines and aminoacids were measured at 298.15K. Based on these data, the adiabatic compressibility coefficients, κ<sub>S</sub>, of solutions were calculated, as well as the hydration numbers of solutes using the concept of Pasynski. It was tested how pH of the system affects the calculated hydration numbers.
It was shown for diluted aqueous solutions of organic non-electrolytes that the effect of solutes on compressibility decrease and the hydration numbers are strongly and directly depending on the length of solute molecules and the groups, which are their constituents.
The results suggest that hydration is an additive parameter, although its mechanisms are different. It seems possible now to predict the hydration numbers of non-electrolytes and compressibility of aqueous solutions of organic non-electrolytes only from their structural formula.
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<li>Kamila KieÅek, Wojciech Marczak, Hydration of non-electrolytes in H<sub>2</sub>O and D<sub>2</sub>O investigated by Passynskiâs method, <i>International Journal of Thermophysics</i> <b>31</b> (2009) 77-84
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