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1Author    Z. Akdeniz, M. P. TosiRequires cookie*
 Title    A Refined Ionic Model for Clusters Relevant to Molten Chloroaluminates  
 Abstract    A model of ionic interactions in neutral and ionized aluminium trichloride clusters, which accounts for ionic deformability through (i) effective valences and (ii) electrostatic and overlap polarizabilities, is evaluated for applications to classical simulation studies of the pure melt and of molten alkali chloroaluminates. The disposable parameters in the model are determined from the measured values of the bond length in the (A1C1 4)~ molecular ion and of an Al-Cl bond length and a vibrational frequency in the A1 2 C1 6 molecular dimer. The model is tested against the remaining available data from experiment and from quantum chemical calculations on molecular bond lengths, bond angles and vibrational frequencies for A1 2 C1 6 , (A1C1 4)~ and (A1 2 C1 7)~ clusters. Structural and dynamical properties are also evaluated for the (A1 2 C1 5) + , A1C1 3 and (A1C1 2) + clusters. The results for the energetics of dissociation, ion transfer and isomer excitation reactions are compared with as yet unpublished data obtained by P. Ballone in first-principles calculations by a density functional method. The overall quality of the tests supports the approximate validity and transferability of the model. 
  Reference    Z. Naturforsch. 54a, 180—186 (1999); received February 17 1999 
  Published    1999 
  Keywords    Ionic Clusters, Liquid Structure, Molten Salts 
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 TEI-XML for    default:Reihe_A/54/ZNA-1999-54a-0180.pdf 
 Identifier    ZNA-1999-54a-0180 
 Volume    54 
2Author    Z. Akdeniz, M. P. TosiRequires cookie*
 Title    Structure and Vibrational Spectra of the Vapour Molecules Fe 2 Cl 6 and AlFeCl 6  
 Abstract    Melting of aluminium and iron trichloride crystals is accompanied by a structural transition from octa-hedral to tetrahedral coordination of the metal ions, and a widely accepted interpretation of their liquid structure is that it mainly consists of strongly correlated dimeric units. Such A1 2 C1 6 and Fe 2 Cl 6 mole-cules are stable in the vapour phase and coexist in gaseous mixtures together with AlFeCl 6 molecules. In this work we extend to Fe 2 Cl 6 and AlFeCl 6 our earlier study of the ionic interactions in A1 2 C1 6], using a model which accounts for ionic deformability through (i) effective valences and (ii) electrostatic and overlap polarizabilities. The main disposable parameters of the model are adjusted to the Fe-Cl bond length in FeCl 3 monomer molecule and to the Fe-Fe bond length and a bond-stretching frequency in the Fe 2 Cl 6 molecule. The results are used to evaluate the structure of the AlFeCl 6 molecule, which has so far only been inferred from the observed Raman spectrum in mixed vapours. Extensive comparisons with data on molecular vibration-al frequencies are also presented for Fe 2 Cl 6 and AlFeCl 6 . 
  Reference    Z. Naturforsch. 54a, 477—481 (1999); received August 3 1999 
  Published    1999 
  Keywords    Ionic Clusters, Molecular Vapours, Molten Salts 
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 TEI-XML for    default:Reihe_A/54/ZNA-1999-54a-0477.pdf 
 Identifier    ZNA-1999-54a-0477 
 Volume    54 
3Author    Masahiko Matsumiya, Masatoshi Takano, Ryuzo Takagi, Reiko FujitaRequires cookie*
 Title    Electrochemical Behavior of Ba 2+ at Liquid Metal Cathodes in Molten Chlorides  
 Abstract    The electrochemcal behavior of Ba 2+ on several liquid metal electrodes (AI, Bi, Cd, Pb, Sn and Zn) in a NaCl-KCl equimolar solvent at 1000 K has been investigated by means of cyclic voltammetry and chronopotentiometry. The kinetic parameters and the diffusion coefficient for Ba 2+ were determined by cyclic voltammetry with conventional, semi-integral, semi-differential methods and chronopotentiometry. It was revealed that on a liquid Pb electrode in the NaCl-KC1 system at 1000 K the quasi-reversible cathodic reaction Ba 2+ + 2e~ + Pb —> BaPb takes place. In addition, the kinetic parameters and the diffusion coefficient agree well with the values determined by various electroanalyses. The possibility of alloy formation between Ba and Sn was also demonstrated in this paper. 
  Reference    Z. Naturforsch. 54a, 739—746 (1999); received September 13 1999 
  Published    1999 
  Keywords    Alloy Formation Reaction, Barium, Liquid Metal Cathodes, Molten Salts 
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 TEI-XML for    default:Reihe_A/54/ZNA-1999-54a-0739.pdf 
 Identifier    ZNA-1999-54a-0739 
 Volume    54 
4Author    Z. Akdeniz, M. Çaliskan, Z. Çiçek, M. P. TosiRequires cookie*
 Title    Polymerie Structures in Aluminium and Gallium Halides  
 Abstract    The anionic species (Al" X3 n+ iwith X = CI or Br and n > 1 have been recognized for a number of years to form in acidic liquid mixtures of aluminium chloride or bromide with the corresponding halides of alkali or organic cations, in relative proportions which vary with the composition of the mixture. In this work we evaluate the structure and the energetics of such polymeric series in a comparative study of Al and Ga compounds. To this end we first extend an earlier study of the ionic interactions in the A1 2 C1 6 molecule] to determine microscopic ionic models for Ga 2 Cl 6 , Al 2 Br 6 , and Ga 2 Br 6 . The models are then used (i) to evaluate the polymeric clusters for n < 4 in the two trivalent-metal chlorides, and (ii) to explore the potential-energy hypersurface of alkali counterions in the case n = 2. We present tests of the results against available data and an evaluation of the convergence of the energy of the polymeric series towards a value of about 0.5 eV per monomer. 
  Reference    Z. Naturforsch. 55a, 575—580 (2000); received February 18 2000 
  Published    2000 
  Keywords    Ionic Clusters, Molecular Vapours, Molten Salts 
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 TEI-XML for    default:Reihe_A/55/ZNA-2000-55a-0575.pdf 
 Identifier    ZNA-2000-55a-0575 
 Volume    55 
5Author    Z. Akdeniz, M. P. TosiRequires cookie*
 Title    Structure and Energetics of Clusters Relevant to Thorium Tetrachloride Melts  
 Abstract    We study within an ionic model the structure and energetics of neutral and charged molecular clusters which may be relevant to molten ThCl 4 and to its liquid mixtures with alkali chlorides, with reference to Raman scattering experiments by Photiadis and Papatheodorou. As stressed by these authors, the most striking facts for ThCl 4 in comparison to other tetrachloride compounds (and in particular to ZrCl 4) are the appreciable ionic conductivity of the pure melt and the continuous structural changes which occur in the melt mixtures with varying composition. After adjusting our model to data on the isolated ThCl 4 tetrahedral molecule, we evaluate (i) the Th 2 Cl 8 dimer and the singly charged species obtained from it by chlorine-ion transfer between two such neutral dimers; (ii) the ThCl 6 and ThCl 7 clusters both as charged anions and as alkali-compensated species; and (iii) various oligomers carrying positive or negative double charges. Our study shows that the characteristic structural properties of the ThCl 4 compound and of the alkali-Th chloride systems are the consequence of the relatively high ionic character of the binding, which is already evident in the isolated ThCl 4 monomer. 
  Reference    Z. Naturforsch. 55a, 772—778 (2000); received August 13 2000 
  Published    2000 
  Keywords    Ionic Clusters, Liquid Structure, Molten Salts 
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 TEI-XML for    default:Reihe_A/55/ZNA-2000-55a-0772.pdf 
 Identifier    ZNA-2000-55a-0772 
 Volume    55 
6Author    Z. Akdeniza, M. P. TosiaRequires cookie*
 Title    Structure and Binding of Ionic Clusters in Th and Zr Chloride Melts  
 Abstract    We discuss microscopic ionic models for the structure and the binding of small clusters which may exist as structural units in molten ThCl4 and ZrCl4 and in their mixtures with alkali halides according to Raman scattering studies of Photiadis and Papatheodorou. The models are adjusted to the two isolated tetrahedral molecules. Appreciably higher ionicity is found for ThCl4 than for ZrCl4, and this fact underlies the strikingly different behaviour of the two systems in the dense liquid state -in particular, a molecular-type structure for molten ZrCl4 against a structure including charged oligomers in molten ThCl4. 
  Reference    Z. Naturforsch. 56a, 717—720 (2001); received September 10 2001 
  Published    2001 
  Keywords    Ionic Clusters, Liquid Structure, Molten Salts 
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 TEI-XML for    default:Reihe_A/56/ZNA-2001-56a-0717.pdf 
 Identifier    ZNA-2001-56a-0717 
 Volume    56 
7Author    S. V. Devyatkin, O. I. Boiko, N. N. Uskova, G. KaptayaRequires cookie*
 Title    Electrochemical Synthesis of Titanium Silicides from Molten Salts  
 Abstract    Presented at the NATO Advanced Study Institute, Kas, Turkey, May 4 -14, 2001. Electrochemical synthesis o f titanium silicides from chloro-fluoride melts has been investigated by thermodynamic calculation, voltammetry and electrolysis. The electrochemical synthesis of four titanium silicides (TiSi2, TiSi, Ti5Si4, Ti5Si3) was to be a one-step process, the stoichiometry of the deposited silicides being correlated with the concentration of Si and Ti ions in the melt. 
  Reference    Z. Naturforsch. 56a, 739—740 (2001); received August 20 2001 
  Published    2001 
  Keywords    Titanium silicides, Electrochemical Synthesis, Molten Salts 
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 TEI-XML for    default:Reihe_A/56/ZNA-2001-56a-0739.pdf 
 Identifier    ZNA-2001-56a-0739 
 Volume    56 
8Author    Alina Wojakowska, Agata GorniakRequires cookie*
 Title    The Electrical Conductivity of Molten (Ag, C d 1/2)B r  
 Abstract    The electrical conductivity of molten (Ag, Cd1/2)Br has been determined as a function of temperature in the whole range of compositions. The resulting activation energy values and the conductivity isotherm at 850 K are compared with those of the system (Ag, C d^^C l. 
  Reference    Z. Naturforsch. 56a, 751—753 (2001); received August 20 2001 
  Published    2001 
  Keywords    AgBr, CdBr2, Molten Salts, Electrical Conductivity 
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 TEI-XML for    default:Reihe_A/56/ZNA-2001-56a-0751.pdf 
 Identifier    ZNA-2001-56a-0751 
 Volume    56 
9Author    C. Herdlicka, J. Richter, M. D. ZeidlerRequires cookie*
 Title    Self-Diffusion in Molten Lithium Nitrate  
 Abstract    Self-diffusion coefficients of 7 Li + ions have been measured in molten LiN0 3 with several com-positions of 6 Li + and 7 Li + over a temperature range from 537 to 615 K. The NMR spin-echo method with pulsed field gradients was applied. It was found that the self-diffusion coefficient depends on the isotopic composition and shows a maximum at equimolar ratio. At temperatures above 600 K this behaviour disappears. 
  Reference    Z. Naturforsch. 47a, 1047—1050 (1992); received July 16 1992 
  Published    1992 
  Keywords    Molten salts, Self-diffusion, Isotope effect, NMR spin-echo 
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 TEI-XML for    default:Reihe_A/47/ZNA-1992-47a-1047.pdf 
 Identifier    ZNA-1992-47a-1047 
 Volume    47 
10Author    Yoshihiro Okamoto, Toru OgawaRequires cookie*
 Title    Structure and Dynamic Properties of Molten Lanthanum Tribromide  
 Abstract    The structure of molten LaBr 3 was investigated by X-ray diffraction and molecular dynamics simu-lations. It was found that the short range structure of molten LaBr 3 is very similar to that of molten LaCl 3 , except for some structural features such as interionic distances based on the difference of anion sizes. In the MD simulation, the shear viscosity of molten LaBr 3 was estimated from the structurally-optimized MD calculations. 
  Reference    Z. Naturforsch. 54a, 91—94 (1999); received November 27 1998 
  Published    1999 
  Keywords    Molten Salt, Rare Earth Halide, X-ray Diffraction, Molecular Dynamics 
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 TEI-XML for    default:Reihe_A/54/ZNA-1999-54a-0091.pdf 
 Identifier    ZNA-1999-54a-0091 
 Volume    54 
11Author    Masahiko Matsumiya, Ryuzo TakagiRequires cookie*
 Title    Electrochemical Impedance Spectroscopic Study on Eu 2+ and Sr 2+ Using Liquid Metal Cathodes in Molten Chlorides  
 Abstract    For the pyrochemical reprocessing of spent metallic nuclear fuels in molten salt baths it is important to investigate the behavior of the electrochemically negative elements Eu and Sr, which are significant fission products. Voltammetric and chronopotentiometric studies have shown that the reduction of Eu 2+ and Sr 2+ on liquid Pb cathodes in molten chloride baths at 1073 K follows the alloy formation reaction: Eu 2+ + 2e~ + 3Pb — • EuPb 3 and Sr 2+ + 2e~ + 3Pb — • SrPb 3 . In the present work these alloy formation reactions were studied by electrochemical impedance spectroscopy. Analysis of the spectra showed that the electronic exchange of Eu 2+ /Eu and Sr 2+ /Sr is quasi-re-versible. Moreover, the experimental results allowed the determination of the kinetic parameters of EU 2+ /EU and Sr 2+ /Sr, the diffusion coefficients of these species in molten chloride baths, and also the diffusion layer thickness. 
  Reference    Z. Naturforsch. 55a, 673—681 (2000); received April 25 2000 
  Published    2000 
  Keywords    Alloy Formation Reaction, Europium, Impedance, Liquid Metal Cathodes, Molten Salts, Strontium 
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 TEI-XML for    default:Reihe_A/55/ZNA-2000-55a-0673.pdf 
 Identifier    ZNA-2000-55a-0673 
 Volume    55 
12Author    Alena Novoselova, Vladimir Shishkin, Vladimir KhokhlovRequires cookie*
 Title    Redox Potentials of Samarium and Europium in Molten Lithium Chloride  
 Abstract    The samarium (III)/(II) and europium (III)/(II) redox potentials in molten lithium chloride were measured using the direct potentiometric method in the temperature range from 923 to 1094 K. Glassy carbon was used as the indifferent working electrode, and the standard chlorine electrode as a reference. The total concentration of rare-earth chlorides dissolved in molten lithium chloride did not exceed 4.5 mol%. 
  Reference    Z. Naturforsch. 56a, 754—756 (2001); received August 20 2001 
  Published    2001 
  Keywords    Molten Salts, Redox Potentials, Samarium Chlorides, Europium Chlorides, Lithium Chloride 
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 TEI-XML for    default:Reihe_A/56/ZNA-2001-56a-0754.pdf 
 Identifier    ZNA-2001-56a-0754 
 Volume    56 
13Author    Roger Blachnik, JohannE. AlbertsRequires cookie*
 Title    Silberhalogenid-Silberchalkogenidsysteme, II Dichten geschmolzener Silberhalogenid-Silberchalkogenidmischungen Silver Halide-Silver Chalcogenide Systems, II Densities of Liquid Silver Halide-Silver Chalcogenide Mixtures  
 Abstract    The densities of liquid mixtures in the systems AgCl-Ag2S, AgCl—Ag2Se, AgCl-Ag2Te, AgBr—Ag2Te, AgJ-Ag2Te and AgJ-Ag2S have been determined as a function of composition and temperature by a dilatometric method. The molvoluminaisotherms of the systems AgJ—Ag2S and AgJ-Ag2Te show negative deviations from ideality, the other systems behave ideally. 
  Reference    (Z. Naturforsch. 31b, 163—166 [1976]; eingegangen am 6. Oktober 1975) 
  Published    1976 
  Keywords    Silver Halide, Silver Chalcogenide, Densities, Molten Salts, Phase Diagram 
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 TEI-XML for    default:Reihe_B/31/ZNB-1976-31b-0163.pdf 
 Identifier    ZNB-1976-31b-0163 
 Volume    31 
14Author    Z. NaturforschRequires cookie*
 Title    The Promotive Properties of Alkali Metal Nitrate Melts for the Partial Oxidation of Methane to Methanol  
 Abstract    B o r-Jih L ee, S higeo K itsu k aw a, S h u k u ji A sa k u ra * , K en z o F u k u d a D epartm ent (Na, K)N 0 3 melts of various ratios were used as prom oters for the partial oxidation of methane to methanol. Experiments were perform ed in a flow reactor system under atmo­ spheric pressure and at various tem peratures in the range of 525-600 °C. The influence of reaction temperature, melt composition, and reduced oxygen species on m ethane conversion and methanol selectivity were investigated systematically. The major reaction products were CH 3O H, CO, C 0 2, and trace amounts of C2H 6 and C2H 4. A m ethane conversion of 1.8-12.4% and a methanol selectivity of 0.4-14.1% were obtained under these reaction condi­ tions. Binary melts could achieve higher m ethanol selectivity than a single melt. The amounts of reduced oxygen species 0 2~ and 0 22-were estimated from thermochemical data according to the ion equilibrium in molten nitrates. The promotive effect of nitrate melts was confirmed and the results indicate that superoxide 0 2~ plays an im portant role for methanol formation. 
  Reference    Z. Naturforsch. 53b, 249—255 (1998); received O ctober 7 1997 
  Published    1998 
  Keywords    Partial Oxidation, Conversion, Selectivity, Molten Salt, Reduced Oxygen Species 
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 TEI-XML for    default:Reihe_B/53/ZNB-1998-53b-0249.pdf 
 Identifier    ZNB-1998-53b-0249 
 Volume    53 
15Author    E. Rejek, J. Richter, A. Stark, M. VogtRequires cookie*
 Title    Ultrasonic Velocity and Absorption in 3 Melts Measured by the Pulse Transmission Method  
 Abstract    (L i,A g)N 0 3, (N a,A g)N O a, (K ,A g)N 0 3, (C s,A g)N 03, (L i,R b)N 0 3, and (N a ,R b)N 0 Ultrasonic velocity and absorption have been measured in molten (L i,A g)N 0 3, (N a,A g)N 03, (K ,A g)N 0 3, (Cs,A g)N03, (L i,R b)N 0 3, and (N a,R b)N 0 3 as functions of composition in the tem­ perature range 230 to 300 °C. An improved pulse transmission device was applied. The obtained accuracy was 2%o for the velocity and 2-4% for the absorption data. The ultrasonic velocity and absorption coefficient (25 MHz) were found to depend linearly on temperature. The dependence of the velocity on the mole fraction could be represented by a cubic polynomial. For the absorption values (referred to the square of frequency) a reasonable general dependence on composition could not be given. The adiabatic compressibility of all mixtures has been calculated from the measured sound velocity. The ratio bulk/shear viscosity and the bulk viscosity itself follow from the measured absorption values together with the velocity values. The conclusion from these data is that ultrasonic absorption in the six investigated systems is governed by the bulk viscosity and that structural rearrangements rather than structural relaxation of the molecules, are the reason for high bulk viscosities in ionic melts. 
  Reference    Z. Naturforsch. 49a, 481—489 (1994); received November 15 1993 
  Published    1994 
  Keywords    Molten salts, Thermophysical properties, Ultrasonic velocities and absorption, Pulse transmission method 
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 TEI-XML for    default:Reihe_A/49/ZNA-1994-49a-0481.pdf 
 Identifier    ZNA-1994-49a-0481 
 Volume    49 
16Author    Yoshihiro Okamoto, Torn OgawaRequires cookie*
 Title    Structure and Thermodynamic Properties of Molten Rare Earth-Alkali Chloride Mixtures  
 Abstract    The dependence of the enthalpy of mixing on the structure of molten rare earth-alkali chloride mixtures has been investigated by molecular dynamics simulation. The experimental enthalpy of the mixing with its negative and its dependence on the cation size was qualitatively reproduced. It became clear that the enthalpy of mixing depends on the structural features of short and medium range. 
  Reference    Z. Naturforsch. 54a, 599—604 (1999); received August 16 1999 
  Published    1999 
  Keywords    Molten Salt, Molecular Dynamics, Enthalpy of Mixing, Rare Earth-alkali Chloride Mixture 
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 TEI-XML for    default:Reihe_A/54/ZNA-1999-54a-0599.pdf 
 Identifier    ZNA-1999-54a-0599 
 Volume    54 
17Author    S. A. Kuznetsov, L. Rycerza, M. Gaune-Escard3Requires cookie*
 Title    Electrochemical and Thermodynamic Properties of EuC13 and EuC12 in an Equimolar NaCl-KCl Melt  
 Abstract    The electroreduction o f EuCl3 in an equimolar NaCl-KCl mixture was studied at 973 -1123 K by different electrochemical methods. This reduction of Eu(III) in NaCl-KCl melt occurs via two successive reversible steps involving transfer o f one and two electrons. The diffusion coefficients of Eu(III) and Eu(II) were measured by linear sweep voltammetry and chronopotentiometry. The values found by these methods are in a good agreement. The standard rate constants for the redox reaction Eu(III) + e~ <=> Eu(II) were calculated from cyclic voltammetry data. The sluggish kinetics of this reaction is discussed in terms o f substantial rearrangement of the europium coordination sphere. Special attention was paid to the choice of working electrodes for the study o f electrode reactions. The formal standard potentials E*E u (^ /Ba, E* eU (hr/eu and the formal redox potentials ^*Eu(ni)/Eu(ii) were determined from open-circuit potentiometry and linear sweep voltammetry data. The free Gibbs energy changes for the reaction EuC13(so1) EuCl2(SO i.) + 1/2 Cl2(g.) and the equilibrium constants o f the metal-salt reaction 2Eu(III) + Eu 3 Eu(II) were calculated. The thermodynamics of the formation o f dilute solutions of europium di-and trichloride in an equimolar NaCl-KCl melt were determined. It was shown that electrochemical transient techniques give the possibility o f the determination of the relative partial molar mixing enthalpy of europium trichloride and dichloride in NaCl-KCl melt. 
  Reference    Z. Naturforsch. 56a, 741 (2001); received August 20 2001 
  Published    2001 
  Keywords    Europium, Molten Salts, Kinetics of Electrode Reaction, Formal Standard Potentials, Mixing Enthalpy 
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 TEI-XML for    default:Reihe_A/56/ZNA-2001-56a-0741.pdf 
 Identifier    ZNA-2001-56a-0741 
 Volume    56 
18Author    AshokK. Adya, Ryuzo Takagi, Marcelle Gaune-EscardRequires cookie*
 Title    Unravelling the Internal Complexities of Molten Salts  
 Abstract    Much experimental and theoretical effort has gone into revealing the internal complexities of molten salts for the past two decades. In this paper we shall show how neutron diffraction and computer sim-ulation techniques have helped in gaining a better understanding of these systems at the microscopic level. Firstly, a short review on the structure of molten halide systems as revealed by these techniques will be presented. Complementarity of using X-rays with neutrons and, some recent results on the struc-ture of molten DyCl 3 obtained by combining neutron and X-ray diffraction with molecular dynamic simulations will be discussed. Neutron diffraction isotopic substitution techniques have played an im-portant role in elucidating the interatomic structure of a diversity of molten salts. Pair distribution func-tions (PDFs), determined for a number of 1:1 and 2 :1 halide melts, provided theorists with a critical test of their model potentials. It is now clear that for 1:1 molten systems theoretical models based on Fumi-Tosi potentials can adequately describe many of the structural features. Nevertheless, the chal-lenge is two fold: (i) to determine real interatomic potentials for 2:1 and 3 :1 molten systems capable of reproducing not only the microscopic structural details obtained at the partial PDF, g a ß (r) level, but also their macroscopic behaviour and, (ii) to characterise the structure in binary molten salt mixtures. 
  Reference    Z. Naturforsch. 53a, 1037—1048 (1998); received November 18 1998 
  Published    1998 
  Keywords    Molten Salts, Structure, Neutron and X-ray Diffraction, Computer Simulations, Liquid State Structural Theory, Molten Halides 
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 TEI-XML for    default:Reihe_A/53/ZNA-1998-53a-1037.pdf 
 Identifier    ZNA-1998-53a-1037 
 Volume    53