Research

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3049 KiB

Open AccessArticle

The Solute-Exclusion Zone: A Promising Application for Mirofluidics

by Chi-Shuo Chen, Erik Farr, Jesse M. Anaya, Eric Y-T Chen and Wei-Chun Chin

Entropy 2015, 17(3), 1466-1476; https://doi.org/10.3390/e17031466 - 23 Mar 2015

Cited by 4 | Viewed by 6071

While unique phenomena exist at fluid-solid phase intersections, many interfacial phenomena manifest solely on limited scales—i.e., the nm-mm ranges—which stifles their application potential. Here, we constructed microfluidic chips that utilize the unique long-distance interface effects of the Solute-Exclusion Zone (EZ) phenomenon [...] Read more.

While unique phenomena exist at fluid-solid phase intersections, many interfacial phenomena manifest solely on limited scales—i.e., the nm-mm ranges—which stifles their application potential. Here, we constructed microfluidic chips that utilize the unique long-distance interface effects of the Solute-Exclusion Zone (EZ) phenomenon to mix, separate, and guide samples in desired directions within microfluidic channels. On our “EZ Chip”, we utilized the interfacial force generated by EZs to transport specimens across streamlines without the need of an off-chip power source. The advantages of easy-integration, low fabrication cost, and no off-chip energy input make the EZ suitable for independent, portable lab-on-chip system applications. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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1956 KiB

Open AccessArticle

Self-oscillating Water Chemiluminescence Modes and Reactive Oxygen Species Generation Induced by Laser Irradiation; Effect of the Exclusion Zone Created by Nafion

by Sergey V. Gudkov, Maxim E. Astashev, Vadim I. Bruskov, Valeriy А. Kozlov, Stanislav D. Zakharov and Nikolai F. Bunkin

Entropy 2014, 16(11), 6166-6185; https://doi.org/10.3390/e16116166 - 21 Nov 2014

Cited by 13 | Viewed by 6346

Abstract

Samples of water inside and outside an exclusion zone (EZ), created by Nafionswollen in water, were irradiated at the wavelength l = 1264 nm, which stimulates the electronic transition of dissolved oxygen from the triplet state to the excited singlet state. This [...] Read more.

Samples of water inside and outside an exclusion zone (EZ), created by Nafionswollen in water, were irradiated at the wavelength l = 1264 nm, which stimulates the electronic transition of dissolved oxygen from the triplet state to the excited singlet state. This irradiation induces, after a long latent period, chemiluminescence self-oscillations in the visible and near UV spectral range, which last many hours. It occurs that this effect is EZ-specific: the chemiluminescence intensity is twice lower than that from the bulk water, while the latent period is longer for the EZ. Laser irradiation causes accumulation of H₂O₂, which is also EZ-specific: its concentration inside the EZ is less than that in the bulk water. These phenomena can be interpreted in terms of a model of decreasing O₂ content in the EZ due to increased chemical activity of bisulfite anions (HSO₃⁻), arisen as the result of dissociation of terminal sulfonate groups of the Nafion. The wavelet transform analysis of the chemiluminescence intensity from the EZ and the bulk water gives, that self-oscillations regimes occurring in the liquid after the latent period are the determinate processes. It occurred that the chemiluminescence dynamics in case of EZ is characterized by a single-frequency self-oscillating regime, whereas in case of the bulk water, the self-oscillation spectrum consists of three spectral bands. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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1131 KiB

Open AccessCommunication

Effect of Atmospheric Ions on Interfacial Water

by Chien-Chang Kurt Kung and Gerald H. Pollack

Entropy 2014, 16(11), 6033-6041; https://doi.org/10.3390/e16116033 - 18 Nov 2014

Cited by 3 | Viewed by 5165

Abstract

The effect of atmospheric positivity on the electrical properties of interfacial water was explored. Interfacial, or exclusion zone (EZ) water was created in the standard way, next to a sheet of Nafion placed horizontally at the bottom of a water-filled chamber. Positive atmospheric [...] Read more.

The effect of atmospheric positivity on the electrical properties of interfacial water was explored. Interfacial, or exclusion zone (EZ) water was created in the standard way, next to a sheet of Nafion placed horizontally at the bottom of a water-filled chamber. Positive atmospheric ions were created from a high voltage source placed above the chamber. Electrical potential distribution in the interfacial water was measured using microelectrodes. We found that beyond a threshold, the positive ions diminished the magnitude of the negative electrical potential in the interfacial water, sometimes even turning it to positive. Additionally, positive ions produced by an air conditioner were observed to generate similar effects; i.e., the electrical potential shifted in the positive direction but returned to negative when the air conditioner stopped blowing. Sometimes, the effect of the positive ions from the air conditioner was strong enough to destroy the structure of interfacial water by turning the potential decidedly positive. Thus, positive air ions can compromise interfacial water negativity and may explain the known negative impact of positive ions on health. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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2827 KiB

Open AccessArticle

Self-Organization at Aqueous Colloid-Membrane Interfaces and an Optical Method to Measure the Kinetics of Exclusion Zone Formation

by Harry Jabs and Beverly Rubik

Entropy 2014, 16(11), 5954-5975; https://doi.org/10.3390/e16115954 - 17 Nov 2014

Cited by 5 | Viewed by 6745

Abstract

Exclusion zone (EZ) formation at water-membrane interfaces was studied via bright- and dark-field microscopy. Various aqueous colloids including suspensions of charged microspheres, silicon dioxide particles, and raw whole milk were studied with Nafion^® hydrophilic membranes. Interfacial formations observed included EZs and more [...] Read more.

Exclusion zone (EZ) formation at water-membrane interfaces was studied via bright- and dark-field microscopy. Various aqueous colloids including suspensions of charged microspheres, silicon dioxide particles, and raw whole milk were studied with Nafion^® hydrophilic membranes. Interfacial formations observed included EZs and more complex patterns including striations, double layers, banding, dendritic aggregates of particles, and double-stranded structures resembling Birkeland current filaments in cold plasmas. A complex three-dimensional dynamic structure and continuous flow patterns persist in and around EZs, maintaining movement of the colloidal particles even after EZs are fully formed, for which a schematic is proposed. Since radiant energy is critical for EZ formation, we hypothesize that these interfacial phenomena are non-equilibrium dissipative structures that self-organize and self-maintain due to ongoing dynamic processes that may involve hydrodynamic interactions. Another experimental approach undertaken involved the construction of a microscope flow cell to measure the kinetics of EZ formation using sequential microphotography analyzed with macro-programmed ImageJ software to investigate effects of different types of conditioned water. No significant difference was found between spring water and the same water treated by a magnetic vortexer. A significant difference was found for municipal tap water compared to electrolyzed alkaline tap water from the same source. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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1325 KiB

Open AccessArticle

The Case for Tetrahedral Oxy-subhydride (TOSH) Structures in the Exclusion Zones of Anchored Polar Solvents Including Water

by Klaus Oehr and Paul H. LeMay

Entropy 2014, 16(11), 5712-5720; https://doi.org/10.3390/e16115712 - 03 Nov 2014

Cited by 1 | Viewed by 6247

Abstract

We hypothesize a mechanistic model of how negatively-charged exclusion zones (EZs) are created. While the growth of EZs is known to be associated with the absorption of ambient photonic energy, the molecular dynamics giving rise to this process need greater elucidation. We believe [...] Read more.

We hypothesize a mechanistic model of how negatively-charged exclusion zones (EZs) are created. While the growth of EZs is known to be associated with the absorption of ambient photonic energy, the molecular dynamics giving rise to this process need greater elucidation. We believe they arise due to the formation of oxy-subhydride structures (OH⁻)(H₂O)₄with a tetrahedral (sp³) (OH⁻)(H₂O)₃ core. Five experimental data sets derived by previous researchers were assessed in this regard: (1) water-derived EZ light absorbance at specific infrared wavelengths, (2) EZ negative potential in water and ethanol, (3) maximum EZ light absorbance at 270 nm ultraviolet wavelength, (4) ability of dimethyl sulphoxide but not ether to form an EZ, and (5) transitory nature of melting ice derived EZs. The proposed tetrahedral oxy-subhydride structures (TOSH) appear to adequately account for all of the experimental evidence derived from water or other polar solvents. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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1813 KiB

Open AccessArticle

A Further Indication of the Self-Ordering Capacity of Water Via the Droplet Evaporation Method

by Igor Jerman and Petra Ratajc

Entropy 2014, 16(10), 5211-5222; https://doi.org/10.3390/e16105211 - 07 Oct 2014

Cited by 3 | Viewed by 5671

Abstract

The droplet evaporation method (DEM) is increasingly used for assessing various characteristics of water. In our research we tried to use DEM to detect a possible self-ordering capability of (spring) water that would be similar to the already found and described autothixotropic phenomenon, [...] Read more.

The droplet evaporation method (DEM) is increasingly used for assessing various characteristics of water. In our research we tried to use DEM to detect a possible self-ordering capability of (spring) water that would be similar to the already found and described autothixotropic phenomenon, namely increasing order of non-distilled water subject to aging. The output of DEM is a droplet remnant pattern (DRP). For analysis of DRP images we used a specially developed computer program that does the frequency distribution analysis of certain parameters of the images. The results of experiments demonstrated statistically significant differences in both aging of water as well as in the glass exposed surface/volume ratio of the aged water. The most important result supporting the self-ordering character of water was found in an increasing dependence between two analyzed parameters: distance and frequency, at the peak frequency. As the result concerns mostly aging and shows increasing order it further corroborates other findings concerning increasing order by aging. Such further confirmation of self-ordering capacity of water is not important only for physical chemistry, but also for biology. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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3866 KiB

Open AccessArticle

Exclusion-Zone Dynamics Explored with Microfluidics and Optical Tweezers

by István N. Huszár, Zsolt Mártonfalvi, András József Laki, Kristóf Iván and Miklós Kellermayer

Entropy 2014, 16(8), 4322-4337; https://doi.org/10.3390/e16084322 - 04 Aug 2014

Cited by 18 | Viewed by 9493

Abstract

The exclusion zone (EZ) is a boundary region devoid of macromolecules and microscopic particles formed spontaneously in the vicinity of hydrophilic surfaces. The exact mechanisms behind this remarkable phenomenon are still not fully understood and are debated. We measured the short- and long-time-scale [...] Read more.

The exclusion zone (EZ) is a boundary region devoid of macromolecules and microscopic particles formed spontaneously in the vicinity of hydrophilic surfaces. The exact mechanisms behind this remarkable phenomenon are still not fully understood and are debated. We measured the short- and long-time-scale kinetics of EZ formation around a Nafion gel embedded in specially designed microfluidic devices. The time-dependent kinetics of EZ formation follow a power law with an exponent of 0.6 that is strikingly close to the value of 0.5 expected for a diffusion-driven process. By using optical tweezers we show that exclusion forces, which are estimated to fall in the sub-pN regime, persist within the fully-developed EZ, suggesting that EZ formation is not a quasi-static but rather an irreversible process. Accordingly, the EZ-forming capacity of the Nafion gel could be exhausted with time, on a scale of hours in the presence of 1 mM Na₂HPO₄. EZ formation may thus be a non-equilibrium thermodynamic cross-effect coupled to a diffusion-driven transport process. Such phenomena might be particularly important in the living cell by providing mechanical cues within the complex cytoplasmic environment. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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1528 KiB

Open AccessArticle

Can the Hexagonal Ice-like Model Render the Spectroscopic Fingerprints of Structured Water? Feedback from Quantum-Chemical Computations

by Javier Segarra-Martí, Daniel Roca-Sanjuán and Manuela Merchán

Entropy 2014, 16(7), 4101-4120; https://doi.org/10.3390/e16074101 - 21 Jul 2014

Cited by 11 | Viewed by 9183

Abstract

The spectroscopic features of the multilayer honeycomb model of structured water are analyzed on theoretical grounds, by using high-level ab initio quantum-chemical methodologies, through model systems built by two fused hexagons of water molecules: the monomeric system [H₁₉O₁₀], in [...] Read more.

The spectroscopic features of the multilayer honeycomb model of structured water are analyzed on theoretical grounds, by using high-level ab initio quantum-chemical methodologies, through model systems built by two fused hexagons of water molecules: the monomeric system [H₁₉O₁₀], in different oxidation states (anionic and neutral species). The findings do not support anionic species as the origin of the spectroscopic fingerprints observed experimentally for structured water. In this context, hexameric anions can just be seen as a source of hydrated hydroxyl anions and cationic species. The results for the neutral dimer are, however, fully consistent with the experimental evidence related to both, absorption and fluorescence spectra. The neutral π-stacked dimer [H₃₈O₂₀] can be assigned as the main responsible for the recorded absorption and fluorescence spectra with computed band maxima at 271 nm (4.58 eV) and 441 nm (2.81 eV), respectively. The important role of triplet excited states is finally discussed. The most intense vertical triplet⇨ triplet transition is predicted to be at 318 nm (3.90 eV). Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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Review

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1071 KiB

Open AccessReview

Illuminating Water and Life

by Mae-Wan Ho

Entropy 2014, 16(9), 4874-4891; https://doi.org/10.3390/e16094874 - 10 Sep 2014

Cited by 12 | Viewed by 25946

Abstract

This paper reviews the quantum electrodynamics theory of water put forward by Del Giudice and colleagues and how it may provide a useful foundation for a new science of water for life. The interaction of light with liquid water generates quantum coherent domains [...] Read more.

This paper reviews the quantum electrodynamics theory of water put forward by Del Giudice and colleagues and how it may provide a useful foundation for a new science of water for life. The interaction of light with liquid water generates quantum coherent domains in which the water molecules oscillate between the ground state and an excited state close to the ionizing potential of water. This produces a plasma of almost free electrons favouring redox reactions, the basis of energy metabolism in living organisms. Coherent domains stabilized by surfaces, such as membranes and macromolecules, provide the excited interfacial water that enables photosynthesis to take place, on which most of life on Earth depends. Excited water is the source of superconducting protons for rapid intercommunication within the body that may be associated with the acupuncture meridians. Coherent domains can also trap electromagnetic frequencies from the environment to orchestrate and activate specific biochemical reactions through resonance, a mechanism for the most precise regulation of gene function. Full article

(This article belongs to the Special Issue Entropy and EZ-Water)

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