Dilution-Induced Physico-Chemical Changes of Metal Oxide Nanoparticles Due to Homeopathic Preparation Steps of Trituration and Succussion

Abstract

Background Although the presence of starting materials in extreme dilutions of homeopathic medicines has been established, the physico-chemical changes of these materials induced by the manufacturing steps—that is, solid–solid mixing involving grinding (trituration) and slurry mixing involving impact (succussion), followed by dilution—are still unknown.

Methods We subjected cupric oxide and zinc oxide nanoparticles (NPs) to the homeopathic processes of trituration and succussion, followed by dilution up to 6 cH. Particle image velocimetry was employed to analyze the fluid motion during succussion and its effect on the NPs. The resulting microstructural and chemical changes at different dilution steps were determined by X-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy and transmission electron microscopy.

Results The succussion triggered multi-sized bubble generation and turbulent fluid motion up to a duration of 400 ms, with maximum average velocity of 0.23 m/s. Due to 1% transfer of kinetic energy from a moving eddy with this velocity, upon collision, the rate of temperature change in a particle of size 1 µm and 1 nm was predicted to rise by approximately 10² K/s and 10⁶ K/s respectively. During trituration, the oxide NPs reduced to metals and did not aggregate by remaining within lactose, but they converted to oxidized finer NPs after impact. Silicate chains leached from the vial cross-linked after third dilution, forming large macro-particles and encapsulating the NPs that were retained and carried at higher dilution steps.

Conclusion The results showed that the NPs sustained significant rate of temperature change due to energy transfer from moving eddies during succussion. Different physico-chemical changes, such as size reduction, successive reduction and oxidation of NPs, and morphological changes, were achieved through trituration and succussion. The retention of NPs within cross-linked poly-siloxane chains reveals the importance of both the borosilicate glass vial and the ethanol solution during preparation of homeopathic medicines.

Keywords

physico-chemical - high dilution - turbulence - nanoparticles - poly-siloxane encapsulation

Highlights

• Physico-chemical changes of nanoparticles were observed after trituration and succussion.

• Succussion involved turbulence generation and bubble formation in the glass vial.

• Rates of temperature rise of 10² K/s and 10⁶ K/s were predicted due to collision of a macro-particle and a nanoparticle, respectively, with a moving eddy during succussion.

• Nanoparticles were reduced after trituration and oxidized after succussion.

• Silicate chains, which were present in different concentrations, leached from the glass vial during succussion.

• Cross-linked poly-siloxane macro-particles encapsulated initial nanoparticles.

• References

• 1 International Organization of Standardization. Microbiology of the food chain. Preparation of test samples, initial suspension and decimal dilutions for microbiological examination — Part 1: General rules for the preparation of the initial suspension and decimal dilutions. Available at: https://www.iso.org . Accessed February 2, 2018
• 2 Halvorson HO, Ziegler NR. Application of statistics to problems in bacteriology: I. A means of determining bacterial population by the dilution method. J Bacteriol 1933; 25: 101-121
• 3 American Public Health Association. Standard methods for the examination of water and wastewater. Available at http://www.standardmethods.org/ . Accessed February 2, 2018
• 4 Inlabtec. Inhomogeneous dilution poses a potential risk to food quality & safety. Available at https://www.inlabtec.com . Accessed February 2, 2018
• 5 Ben-David A, Davidson CE. Estimation method for serial dilution experiments. J Microbiol Methods 2014; 107: 214-221
• 6 Linder RE, Strader LF, McElroy WK. Measurement of epididymal sperm motility as a test variable in the rat. Bull Environ Contam Toxicol 1986; 36: 317-324
• 7 Mandzy N, Grulke E, Druffel T. Breakage of TiO₂ agglomerates in electrostatically stabilized aqueous dispersions. Powder Technol 2005; 160: 121-126
• 8 Liu Z, Hitimana E, Olsen MG, Hill JC, Fox RO. Turbulent mixing in the confined swirling flow of a multi-inlet vortex reactor. AIChE J 2017; 63: 2409-2419
• 9 Basu A, Suresh AK, Kane SG, Bellare JR. A review of machines and devices to potentize homeopathic medicines. Homeopathy 2017; 106: 240-249
• 10 Hahnemann S. Essay on a new principle for ascertaining the curative powers of drugs. Hufeland's Journal 1796; 2: 295-352
• 11 Endler P, Schulte J. Ultra High Dilution. Physiology and Physics. The Netherlands: Springer; 2013
• 12 Davenas E, Beauvais F, Amara J. , et al. Human basophil degranulation triggered by very dilute antiserum against IgE. Nature 1988; 333: 816-818
• 13 Chaplin MF. The memory of water: an overview. Homeopathy 2007; 96: 143-150
• 14 Teixeira J. Can water possibly have a memory? A sceptical view. Homeopathy 2007; 96: 158-162
• 15 Rao ML, Roy R, Bell IR, Hoover R. The defining role of structure (including epitaxy) in the plausibility of homeopathy. Homeopathy 2007; 96: 175-182
• 16 Roy R, Tiller WA, Bell I, Hoover MR. The structure of liquid water; novel insights from materials research; potential relevance to homeopathy. Mater Res Innov 2005; 9: 98-103
• 17 Anagnostatos GS. Small water clusters (Clathrates) in the homoeopathic preparation process. In: Endler PC, Schulte J. , eds. Ultra High Dilution–Physiology and Physics. Dordrecht, The Netherlands: Kluwer Academic Publishers; 1994: 121-128
• 18 Walach H, Jonas WB, Ives J, van Wijk R, Weingärtner O. Research on homeopathy: state of the art. J Altern Complement Med 2005; 11: 813-829
• 19 Anick DJ, Ives JA. The silica hypothesis for homeopathy: physical chemistry. Homeopathy 2007; 96: 189-195
• 20 Chikramane PS, Kalita D, Suresh AK, Kane SG, Bellare JR. Why extreme dilutions reach non-zero asymptotes: a nanoparticulate hypothesis based on froth flotation. Langmuir 2012; 28: 15864-15875
• 21 Chikramane PS, Suresh AK, Bellare JR, Kane SG. Extreme homeopathic dilutions retain starting materials: a nanoparticulate perspective. Homeopathy 2010; 99: 231-242
• 22 Sur I, Cam D, Kahraman M, Baysal A, Culha M. Interaction of multi-functional silver nanoparticles with living cells. Nanotechnology 2010; 21: 175104
• 23 Bhattacharyya SS, Mandal SK, Biswas R. , et al. In vitro studies demonstrate anticancer activity of an alkaloid of the plant Gelsemium sempervirens. Exp Biol Med (Maywood) 2008; 233: 1591-1601
• 24 Schmidt JM. History and relevance of the 6th edition of the Organon of Medicine (1842). Br Homoeopath J 1994; 83: 42-48
• 25 Elia V, Baiano S, Duro I, Napoli E, Niccoli M, Nonatelli L. Permanent physico-chemical properties of extremely diluted aqueous solutions of homeopathic medicines. Homeopathy 2004; 93: 144-150
• 26 Torres JL. On the physical basis of succussion. Homeopathy 2002; 91: 221-224
• 27 Raffel M, Willert CE, Scarano F, Kähler CJ, Wereley ST, Kompenhans J. Particle Image Velocimetry: A Practical Guide. Springer; 2018
• 28 Melling A. Tracer particles and seeding for particle image velocimetry. Meas Sci Technol 1997; 8: 1406-1416
• 29 Smith MR, Donnelly RJ, Goldenfeld N, Vinen WF. Decay of vorticity in homogeneous turbulence. Phys Rev Lett 1993; 71: 2583-2586
• 30 Iyer CO, Ceccio SL. The influence of developed cavitation on the flow of a turbulent shear layer. Phys Fluids 2002; 14: 3414-3431
• 31 Vassilicos JC. Dissipation in turbulent flows. Annu Rev Fluid Mech 2015; 47: 95-114
• 32 Tanahashi M, Kang SJ, Miyamoto T, Shiokawa S, Miyauchi T. Scaling law of fine scale eddies in turbulent channel flows up to Reτ=800. Int J Heat Fluid Flow 2004; 25: 331-340
• 33 Yu J, Ran J. Facile preparation and enhanced photocatalytic H₂-production activity of Cu(OH)₂ cluster modified TiO_2. . Energy Environ Sci 2011; 4: 1364-1371
• 34 Ghijsen J, Tjeng LH, Eskes H. , et al. Electronic structure of Cu₂O and CuO. Phys Rev B Condens Matter 1988; 38: 11322-11330
• 35 Poulston S, Parlett P, Stone P, Bowker M. Surface oxidation and reduction of CuO and Cu₂O studied using XPS and XAES. Surf Interface Anal 1996; 24: 811-820
• 36 Alexander MR, Short R, Jones F, Michaeli W, Blomfield C. A study of HMDSO/O₂ plasma deposits using a high-sensitivity and-energy resolution XPS instrument: curve fitting of the Si 2p core level. Appl Surf Sci 1999; 137: 179-183
• 37 Mehta BM, Deeth HC. Blocked lysine in dairy products: formation, occurrence, analysis, and nutritional implications. Compr Rev Food Sci Food Saf 2016; 15: 206-218
• 38 Wang N, Hsu C, Zhu L, Tseng S, Hsu JP. Influence of metal oxide nanoparticles concentration on their zeta potential. J Colloid Interface Sci 2013; 407: 22-28
• 39 Arukalam IO, Oguzie EE, Li Y. Nanostructured superhydrophobic polysiloxane coating for high barrier and anticorrosion applications in marine environment. J Colloid Interface Sci 2018; 512: 674-685
• 40 Sun X, Turnage S, Iezzi EB. , et al. Water permeation and corrosion resistance of single-and two-component hydrophobic polysiloxane barrier coatings. J Coat Technol Res 2017; 14: 1247-1258
• 41 Savage SB. Laminar radial flow between parallel plates. J Appl Mech 1964; 31: 594-596
• 42 Carling PA, Perillo M, Best J, Garcia MH. The bubble bursts for cavitation in natural rivers: laboratory experiments reveal minor role in bedrock erosion. Earth Surf Process Landf 2017; 42: 1308-1316
• 43 Bartos C, Kukovecz Á, Ambrus R, Farkas G, Radacsi N, Szabó-Révész P. Comparison of static and dynamic sonication as process intensification for particle size reduction using a factorial design chemical engineering and processing: process intensification. Chem Eng Process 2015; 87: 26-34
• 44 Patil MN, Pandit AB. Cavitation--a novel technique for making stable nano-suspensions. Ultrason Sonochem 2007; 14: 519-530
• 45 Raman V, Abbas A. Experimental investigations on ultrasound mediated particle breakage. Ultrason Sonochem 2008; 15: 55-64
• 46 Kiel S, Grinberg O, Perkas N, Charmet J, Kepner H, Gedanken A. Forming nanoparticles of water-soluble ionic molecules and embedding them into polymer and glass substrates. Beilstein J Nanotechnol 2012; 3: 267-276
• 47 Yusof NSM, Babgi B, Alghamdi Y, Aksu M, Madhavan J, Ashokkumar M. Physical and chemical effects of acoustic cavitation in selected ultrasonic cleaning applications. Ultrason Sonochem 2016; 29: 568-576
• 48 Holandino C, Oliveira AP, Homsani F. , et al. Structural and thermal analyses of zinc and lactose in homeopathic triturated systems. Homeopathy 2017; 106: 160-170
• 49 Sarkar T, Konar A, Sukul NC, Sohel Md A, Sengupta A, Sukul A. DSC reveals variation in enthalpy associated with free water molecules in water ethanol solution exposed to x-rays and magnetic field. Clin Experimental Homeopathy 2017; 4: 50-78
• 50 Temgire MK, Suresh AK, Kane SG, Bellare JR. Establishing the interfacial nano-structure and elemental composition of homeopathic medicines based on inorganic salts: a scientific approach. Homeopathy 2016; 105: 160-172
• 51 Ives JA, Moffett JR, Arun P. , et al. Enzyme stabilization by glass-derived silicates in glass-exposed aqueous solutions. Homeopathy 2010; 99: 15-24