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Abstract  

An extensive thermodynamic study has been carried out on aqueous solutions, obtained through the iteration of two processes: a dilution 1:100 in mass and a succussion. The iteration is repeated until extreme dilutions are reached (less than 1⋅10–5 mol kg–1 ) to the point that we may call the resulting solution an 'extremely diluted solution'. We conducted a calorimetric study, at 25C, of the interaction of those solutions with acids or bases. Namely, we measured the heats of mixing of acid or basic solutions with bidistilled water and compared them with the analogous heats of mixing obtained using the 'extremely diluted solutions'. Despite the extreme dilution of the latter solutions, we found a relevant exothermic excess heat of mixing, excess with respects to the corresponding heat of mixing with the untreated solvent. Such an excess has been found in about the totality of measurements, and of a magnitude being well beyond one that could arise any issue of sensibility of the instrumental apparatus. Here we thus show that successive dilutions and succussions can permanently alter the physico-chemical properties of the solvent water. The nature of the phenomena here described still remains unexplained, nevertheless some significant experimental results were obtained.

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Abstract  

The extremely diluted solutions are anomalous solutions obtained through the iteration of two processes: a dilution 1:100 in mass and a succussion. The iteration is repeated until extreme dilutions are reached (less than 110-5mol kg-1) to the point that we may call the resulting solution an extremely diluted solution, namely the composition of the solution is identical to that of the solvent used (e.g. twice distilled water). We conducted thermodynamic and transport measurements of the solutions and of the interaction of those solutions with acids or bases. The purpose of this study is to obtain information about the influence of successive dilutions and succussions on the water structure of the solutions under study. We measured the heats of mixing of acid or basic solutions with such extremely diluted solutions, their electrical conductivity and pH, comparing with the analogous heats of mixing, electrical conductivity and pH of the solvent. We found some relevant exothermic excess heats of mixing, higher electrical conductivity and pH than those of the untreated solvent. The measurements show a good correlation between independent physico-chemical parameters. Care was taken to take into account the effect of chemical impurities deriving from the glass containers. Here we thus show that successive dilutions and succussions can permanently alter the physico-chemical properties of the water solvent. The nature of the phenomena here described still remains unexplained, nevertheless some significant experimental results were obtained.

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Abstract  

An extensive study has been carried out on extremely diluted aqueous solutions (EDS). These solutions revealed a really intriguing physico-chemical behaviour, characterized by multiple independent variables. Because of their behaviour, EDS can be described as far-from-equilibrium systems, capable of self-organization as a consequence of little perturbations. In this paper we investigate the stability of the calorimetric behaviour of EDS with a high ionic force, due to the presence of the sodium chloride electrolyte. We measured the excess heats of mixing of EDS with basic solutions, both with and without a high concentration of NaCl, and compared the results. In particular, we explored these concentrations: 0.5 and 1Mmol kg−1). The analysis of the experimental results shows that the calorimetric response of the EDS is stable when they are in a concentrated solution of NaCl. That is of great relevance for the eventual pharmacological action of these solutions, since it involves the interaction with fluids of complex chemical composition and high concentration.

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A miniaturized effusion cell adapted to a Sorption LKB microcalorimeter has been designed, built and tested. Vaporization is performed isothermally into a vacuum through a small orifice permitting a vapour pressure very close to the equilibrium values. The cell has been tested by measuring the enthalpies of vaporization at 298.15 K of reference liquid compounds (water, benzene, propanol-1, propanol-2) with a reproducibility better than 1%. Enthalpies of vaporization of butanol-1 and deuterated water have also been determined.

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A model for the interactions involving hydrophilic structure maker solutes

A thermodynamic study of ternary aqueous solutions of glucose and hydroxylated substances

Journal of Thermal Analysis and Calorimetry
Authors: Giuseppina Castronuovo, V. Elia, and Filomena Velleca

Enthalpies of dilution of ternary aqueous solutions containing glucose and alkan-1-ols, alkan-1,2-diols and alkan-m,n-diols were determined at 298.15 K by flow microcalorimetry. The pair-wise cross interaction coefficients of the virial expansion of the excess enthalpies were evaluated: they are positive and depend in a complex manner on the length of the alkyl chain of the alkanols. The behaviour of these systems is interpreted in terms of preferential interactions between the hydrophilic groups of the alkanols and the destructured domain present on glucose.

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Abstract

Conductometric and calorimetric titrations of Extremely Diluted Solutions (EDS) were performed by adding HCl or NaOH solutions. The aim of this study is to obtain further confirmation of the hypothesized presence, in the EDS, of molecular aggregates of water molecules. The measurements on the EDS evidenced some relevant differences compared to those on solutions with just water as solvent. The conductivity and the pH caused by adding the titrant, namely NaOH or HCl, were markedly different to those of the control solutions. We suppose that the preparation procedure of the EDS could produce non-equilibrium changes in the supramolecular structure of water. The experimental results were interpreted by considering the interactions that can take place between the OH or H3O+ and the hypothesized molecular aggregates of water molecules i.e. dissipative structures. A comparison was made about the nature of the driving force that leads to the formation of the complexes between the two ions deriving from probes and the molecular aggregates of water molecules (dissipative structures). In this study, we have determined the thermodynamic parameters of association between molecular aggregates of water molecules (dissipative structures) in the EDS and OH or H3O+ probe ions. The experimental results were interpreted by considering a favorable interaction between the H3O+ and OH ions and the dissipative structures, due, probably, to steric hindrance and chemical affinity with the aggregates.

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Aqueous nanostructures in water induced by electromagnetic fields emitted by EDS

A conductometric study of fullerene and carbon nanotube EDS

Journal of Thermal Analysis and Calorimetry
Authors: V. Elia, L. A. Marrari, and E. Napoli

Abstract

This article reports the experimental results of a conductometric study on the time evolution, over a 541-day period, of 450 samples of Extremely Diluted Solutions (EDS) of fullerene and carbon nanotube and 450 samples of twice-distilled water, stored in alternate rows of EDS and water spaced 0.5 cm apart. The purpose was to establish whether these two aqueous systems are able to transmit, via electromagnetic fields, their variations in the supramolecular structure of the solvent water which has not undergone any previous perturbation. The chemical-physical method employed was conductometry, which proved to be the simplest and most efficient means for quickly and accurately monitoring the structural variations. In addition, since it has been demonstrated that there is a clear linear correlation between specific conductivity and heat of mixing with alkaline solutions, the conductometric result can also be extended to the calorimetric result. These findings, though doubtless unexpected and intriguing, are highly significant. The alterations over time of the pure water samples follow those of the EDS surprisingly closely.

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Conductometric and calorimetric studies of the serially diluted and agitated solutions

On the combined anomalous effect of time and volume parameters

Journal of Thermal Analysis and Calorimetry
Authors: P. Belon, V. Elia, L. Elia, M. Montanino, E. Napoli, and M. Niccoli

Abstract  

We systematically analysed the experimental data related to the specific conductivities and heats in excess of several serially diluted and agitated solutions (SDA for short). For all of the analysed samples, we found that both the excess conductivity, χE (μS cm−1), and excess heat, Q mix E (J kg−1), varied with the age of the sample (up to 2 years of ageing). Furthermore, we found that after a certain period of ageing, small volume samples exhibited a much higher excess than large volume ones. The results we report in this paper are the product of a systematic study, during which we operated on known and constant volumes across the life of the samples. The incidence of volume on χE and Q mix E turned out to be overwhelming when compared with that of time. The temporal evolution of the smaller samples was found significantly higher than that of the larger volume ones. A careful numerical analysis of the results uncovered an extraordinary and unexpected correlation, of exponential kind, between the excess parameters and the volume of the solution in the container. As for the temporal evolution of these systems, we found that the measured excess heats and conductivity often reach a maximum. That led us to the conclusion that the temporal evolution of the physico-chemical parameters is not caused by the slow process of equilibrium attainment; on the contrary, these systems are far from equilibrium systems, dissipative structures, whose experimental behaviour is certainly due to the variation of the super-molecular structure of the solvent, water. The agitation phase during the preparation could be the trigger for the formation of dissipative structures and the emergence of the novel behaviour. We put forth a simple rationalizing hypothesis, based on the general idea of water as an auto-organizing system that, when elicited by even small perturbations, can enter a far from equilibrium state, sustained by the dissipation of the electromagnetic energy coming from the environment. (Dissipative Structures).

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Abstract  

An extensive study has been carried out on aqueous ‘extremely diluted solutions’ (EDS). The employed experimental methodologies were well established physico-chemical techniques: flux calorimetry, conductometry, pH-metry, e.m.f. of suitable galvanic cell. The obtained results show that the preparation procedure significantly alters the physico-chemical behaviour of such solutions. Moreover, the analysis of the experimental data vs. the ‘arrow of time’ turned out to be astonishingly important. In fact some measured physico-chemical parameters evolve with time. Some experimentally measurable physico-chemical properties of the solvent water were largely affected by both time and the ‘life path’ of the samples. In particular, we evidenced two new experimental phenomena characterizing the EDS: the presence of a series of maximums in the measured electrical conductivity vs. the sample age; the dependence of said maximums on the volume of the EDS during its ageing. All of these new experimental results clearly suggest the presence of an extended and ‘ordered’ dynamics involving the whole of the water molecules in the liquid. A temporal evolution, featuring three maximums in the course of four years of ageing and the dependence on the ageing volumes do not fit the framework of classical thermodynamics. It therefore seems appropriate to interpret these phenomena on the basis of the thermodynamics of dissipative structures, which are far from equilibrium systems.

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‘Extremely diluted solutions’ as multi-variable systems

A study of calorimetric and conductometric behaviour as a function of the parameter time

Journal of Thermal Analysis and Calorimetry
Authors: V. Elia, L. Elia, P. Cacace, E. Napoli, M. Niccoli, and F. Savarese

Abstract  

A large number of thermodynamic and transport measurements were conducted on ‘extremely diluted solutions’ (EDS). The physico-chemical results presented here allow us to hypothesize that the process of iterated dilutions and succussions is capable of modifying in a permanent way the features of water. A really intriguing phenomenon was the evolution of two physico-chemical properties with time. The calorimetric and conductometric measures were carried out as a function of the age of the samples. We found a good linear correlation between these two independent parameters, also as a function of time. A careful study of the phenomenon puts in evidence that these solutions are characterised by multiple independent variables. The EDS behave as complex systems, influenced by peculiar aspects of the preparation technique and also by the storage conditions. The EDS are far-from-equilibrium systems, capable of auto-organising themselves as a consequence of little perturbations.

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