Degree Of Solvation Research Articles

Unveiling the Factors Influencing Different Nucleation Pathways and Liquid-Liquid Phase Separation.

Exploring nucleation pathways has been a research hot spot in the fields of crystal engineering. In this work, vanillin as a model compound was utilized to explore the factors influencing different nucleation pathways with or without liquid-liquid phase separation (LLPS). A thermodynamic phase diagram of vanillin in the mixed solvent system of water and acetone from 10 to 55 °C was determined. It was found that the occurrence of LLPS might be related to different nucleation pathways. Under the guidance of a thermodynamic phase diagram, Raman spectroscopy and molecular simulation were applied to investigate the influencing factors of different nucleation paths. It was found that the degree of solvation is a key factor determining the nucleation path, and strong solvation could lead to LLPS. Additionally, the molecular self-assembly evolution during the crystallization process was further investigated by using small-angle X-ray scattering (SAXS) and dynamic light scattering (DLS). The findings indicate that larger clusters with a diffuse transition layer may lead to LLPS during the nucleation process.

Electrochemical Amalgamation Optimization as Part of the Development of the OREATE Process

Oxide reduction by electrochemical amalgamation and thermal extraction (OREATE) is an electrochemical process in which metal oxides are converted to highly pure metals. This process that is currently being developed at LANL involves the dissolution and chlorination of the metal oxide into an acidic medium. This metal cation is then electrochemically amalgamated via reduction using a mercury pool cathode. Finally, mercury's high vapor pressure allows an easy thermal extraction process to obtain the metal. In addition to its ability to electrochemically form amalgams, mercury is used because it has a high hydrogen evolution overpotential, allowing for a higher current efficiency for reduction of the metals in acidic solution. As a critical step of the OREATE process, the electrochemical amalgamation reaction must be optimized in order to advance the overall performance.In this work, we studied the electrochemical amalgamation of cerium through anodic stripping voltammetry (ASV) experiments using a silver-based mercury film electrode (SBMFE). The SBMFE allows for the electrochemical amalgamation to be optimized at a smaller scale than the mercury pool, which not only minimizes the amount of mercury needed, but also drastically reduces the experiment time. This study included several different experimental parameters such as the pH of the buffered solution, concentration of cerium, reduction potential, and temperature. For each parameter, the reaction rate and current efficiency were evaluated to determine the optimal conditions for the electrochemical amalgamation reaction.The results showed that the pH of the buffered solution must be 3.5 or lower to avoid the formation of cerium hydroxides, which can passivate the surface of the mercury electrode. However, an increasingly acidic solution promotes the hydrogen evolution reaction, which directly competes with the electrochemical reduction of cerium, decreasing the overall current efficiency. Likewise, it has been demonstrated that an increase of the cerium concentration in solution drops the current efficiency of the electrochemical amalgamation reaction. This effect can be explained by the fact that cerium is a small cation with a +3 charge that leads to a high degree of solvation. Therefore, as the cerium concentration in solution increases, more water molecules are brought to the electrode surface during electrochemical amalgamation. This favors the water reduction reaction that increases hydrogen evolution and lowers current efficiency. However, increasing the concentration of cerium enhances the reaction rate of the electrochemical amalgamation, resulting in more cerium entering the mercury film. Furthermore, as the reduction potential is moved towards more negative potentials, the reaction rate increases. However, a more negative reduction potential promotes a faster hydrogen evolution reaction, which diminishes the current efficiency. Finally, it has been demonstrated that temperature increases the reaction rate, though it does not have a significant effect on the current efficiency.In conclusion, a variety of system parameters were explored for their effect on current efficiency and reaction rate of the electrochemical amalgamation reaction. This allowed for the determination of the optimal parameters to be used during the electrochemical amalgamation in the large-scale OREATE process.

Roles of H-Bonding and Hydride Solvation in the Reaction of Hydrated (Di)electrons with Water to Create H2 and OH.

Even though single hydrated electrons (ehyd-'s) are stable in liquid water, two hydrated electrons can bimolecularly react with water to create H2 and hydroxide: ehyd- + ehyd- + 2H2O → H2 + 2OH-. The rate of this reaction has an unusual temperature and isotope dependence as well as no dependence on ionic strength, which suggests that cosolvation of two electrons as a single hydrated dielectron (e2,hyd2-) might be an important intermediate in the mechanism of this reaction. Here, we present an ab initio density functional theory study of this reaction to better understand the potential properties, reactivity, and experimental accessibility of hydrated dielectrons. Our simulations create hydrated dielectrons by first simulating single ehyd-'s and then injecting a second electron, providing a well-defined time zero for e2,hyd2- formation and offering insight into a potential experimental route to creating dielectrons and optically inducing the reaction. We find that e2,hyd2- immediately forms in every member of our ensemble of trajectories, allowing us to study the molecular mechanism of H2 and OH- formation. The subsequent reaction involves separate proton transfer steps with a generally well-defined hydride subintermediate. The time scales for both proton transfer steps are quite broad, with the first proton transfer step spanning times over a few ps, while the second proton transfer step varies over ∼150 fs. We find that the first proton transfer rate is dictated by whether or not the reacting water is part of an H-bond chain that allows the newly created OH- to rapidly move by Grotthuss-type proton hopping to minimize electrostatic repulsion with H-. The second proton transfer step depends significantly on the degree of solvation of H-, leading to a wide range of reactive geometries where the two waters involved can lie either across the dielectron cavity or more adjacent to each other. This also allows the two proton transfer events to take place either effectively concertedly or sequentially, explaining differing views that have been presented in the literature.

Intra-strand phosphate-mediated pathways in microsolvated double-stranded DNA

We argue that dry DNA charge transport in molecular junctions, over distances of tens of nanometers, can take place via independent intra-strand pathways involving the phosphate groups. Such pathways explain recent single-molecule experiments that compare currents in intact and nicked 100 base-pair double-stranded DNA. We explore the conditions that favor independent intra-strand transport channels with the participation of the phosphate groups, as opposed to purely base-mediated transport involving the pi-stacked bases and inter-strand transitions. Our computations demonstrate how long-distance transport pathways in DNA are tuned by the degree of solvation, which affects the level of dynamic disorder in the pi-stacking, and the energies of phosphate-group molecular orbitals.

Exploring metal carbamates as precursors for the synthesis of metal-organic frameworks.

In the synthesis of metal-organic frameworks (MOFs), the choice of the metal precursor plays a key role because of the influence that it can exert on the crystallization kinetics. The present work explores the use of metal-carbamato complexes for the synthesis of benchmark MOFs, namely HKUST-1 and UiO-66. Cu2(O2CNEt2)4·2NHEt2 and Zr(O2CNEt2)4, prepared using straightforward CO2 fixation reactions starting from the corresponding metal chlorides and diethylamine, were employed as metal precursors for MOF formation. The synthesis conditions, including the solvent, temperature, and ligand protonation degree, were systematically investigated, revealing metal carbamates as highly reactive precursors due to their prompt release of CO2 and amine upon reaction with protic species, i.e., the polycarboxylic linkers. This property of metal carbamates allowed us to identify room temperature protocols to achieve MOFs with comparable properties to those obtained using traditional metal precursors. Subsequent optimization of the reaction conditions led to the design of a one-pot synthetic strategy for HKUST-1, starting directly from copper(II) chloride and diethylamine under a CO2 atmosphere. The MOFs were characterized using various techniques, including powder X-ray diffraction, N2 sorption analysis, 1H nuclear magnetic resonance spectroscopy, and CHN elemental analysis, and compared to reference samples prepared according to literature procedures.

ATR FTIR spectroscopy of protein and surfactant adsorption to the oil-water interface

An oil-infused polyelectrolyte multilayer (PEM) immersed in aqueous solution is a valid mimic for an oil-water interface, that can be used to probe adsorption of surfactants (including co-/competitive adsorption) using attenuated total reflection Fourier transform infrared spectroscopy (ATR FTIR). A PEM has been formed on an ATR internal reflection element, dried and then re-solvated with oil, then exposed to a flowing solution of protein, and subsequently a solution of surfactant. The PEM had undergone prior characterization with atomic force microscopy (AFM). The experiment was replicated using profile analysis tensiometry (PAT). The PEM displays a high degree of solvation with oil; it retains most of this oil in the presence of flowing aqueous solution. FTIR spectra confirmed adsorption of a dairy protein (β-lactoglobulin) to the medium chain triglyceride (MCT)-water interface, and the response of the adsorbed protein layer to a common food formulation surfactant (Tween 60) in the aqueous phase above the interface. The protein is observed to adsorb strongly and irreversibly to the MCT oil-water interface, and the Tween 60 molecules are seen to co-adsorb rather than displace the protein. This observation is supported by measurements of sequential co-adsorption undertaken with PAT.

An analytical study to verify the suitability of free and gelled siloxanes for the treatment of modern oil paintings

Since its introduction, about 15 years ago, the cyclic siloxane Cyclomethicone D5 has become increasingly used in the conservation of Cultural Heritage. In free form it allows the temporary hydrophobization of sensitive surfaces that must be treated in an aqueous environment; in the commercially available gelled form it allows the formulation of water-in-oil particle emulsions for surface cleaning or removal of film-forming substances, depending on the conditions of the aqueous phase. Over time, doubts have arisen about the real inertness of this solvent towards modern oil media. In addition, European regulations have restricted its use in consideration of its environmental impact, and so the already difficult availability of the material could further complicate; this advises the search for a substitute solvent. These two arguments motivated this study, conducted on two modern oil paintings: one unvarnished on paper, the other varnished on canvas. Samples of these paintings were treated under different conditions with D5 and the potential substitute chosen: dodecamethylpentasiloxane. The GC–MS and SEM-EDS analysis of the treated samples made it possible to evaluate and compare the degree of interaction with the oil binder in terms of leaching and topographic alterations of the surface, for both the free solvents and their gelled forms. Tests conducted on specially prepared paint samples also made it possible to evaluate the degree of solvation and consequent swelling produced by the two solvents on the different binders.

Hydration sphere structure of architectural molecules: Polyethylene glycol and polyoxymethylene oligomers

Non-toxic, chemically inert, organic polymers as polyethylene glycol (PEG) and polyoxymethylene (POM) have versatile applications in basic research, industry and pharmacy. In this work, we aim to characterize the hydration structure of PEG and POM oligomers by exploring how the solute disturbs the water structure compared to the bulk solvent and how the solute chain interacts with the solvent. We explore the effect of (i) the C–C–O (PEG) versus C-O (POM) constitution of the chain and (ii) chain length. To this end, MD simulations followed by clustering and topological analysis of the hydration network, as well as quantum mechanical calculations of atomic charges are used.We show that the hydration varies with chain conformation and length. The degree of folding of the chain impacts its degree of solvation, which is measurable by different parameters as for example the number of water molecules in the first solvation shell and the solvent accessible surface. Atomic charges calculated on the oligomers in gas phase are stable throughout conformation and chain length and seem not to determine solvation. Hydration however induces charge transfer from the solute molecule to the solvent, which depends on the degree of hydration.

Electrochemical insights into the energy storage mechanism of birnessite in aqueous solutions

The birnessite structure of manganese dioxide makes this compound a promising electrode materials for energy storage devices including, in particular for supercapacitors, thanks to the high theoretical capacitance and pseudocapacitive response of MnO2. The effect of ionic species, in particular alkali cations, on the structure of birnessite has been intensively discussed, however their role on the charge storage mechanism is still controversial. Taking into consideration the solvation/desolvation process of different alkali cations (Li+, Na+, K+ and Cs+), this work unveils relevant new aspects of the pseudocapacitive charge storage mechanism of birnessite. The work also discusses the simultaneous contribution of non-faradaic (double-layer processes) and faradaic redox reactions to the charge storage mechanism based on electrochemical impedance spectroscopy (EIS) analysis. It was found that the relative extension of these processes was dependent on diffusional features related to the cation degree of solvation. Results revealed that the potassium birnessite exhibited an interesting specific capacitance value that reached 175.6 F g−1 at 0.5 A g−1 in a potential window of 0.8 V in 0.5 M Li2SO4. This capacitance value includes a contribution resulting from intercalation/deintercalation of cations in the interlayer region and a larger contribution from the double-layer processes (above 76%). This investigation provides new electrochemical insights on the charge storage of birnessite, highlighting the role of alkali ions intercalation in the interlayer structure of birnessite.

Entropic Effects on the Aqueous Microsolvation of Protonated Glycine and Protonated β-Alanine. Hybrid Density Functional Theory Born-Oppenheimer Molecular Dynamics Studies.

Recent low-temperature infrared-based experimental studies provided information about the effects of aqueous microsolvation on the intramolecular hydrogen bond of protonated glycine and β-alanine [J. Phys. Chem. A 2019, 123, 3355]. Here we address the temperature-dependent entropic effects on the aqueous microsolvation patterns of these protonated amino acids using the AAH+(H2O)n (n = 1-8) cluster model at 50 K and room temperature with Born-Oppenheimer molecular dynamics using a calibrated hybrid density functional. The CCOOH-Ow, N-Ow, and center-of-mass-Ow radial distribution functions provide accurate structural data and temperature-dependent water coordination numbers vs. solvation degree. The solvation patterns for protonated glycine at 50 K show structural features in agreement with previous static optimizations. However, entropic effects at room temperature play a crucial role in the evolution of the intramolecular HB strength vs. solvation degree for both protonated amino acids. With increasing hydration entropic effects favor the making of solvent hydrogen bond networks over full solvation of protonated glycine. At room temperature four water molecules are needed to build the first solvation shell for protonated glycine while five are required for protonated β-alanine. A new statistical Cumulative Percentage of Structures (CPS) scheme is proposed; when the CPS data are analyzed in light of the empirical formula of Rozenberg et al. [Phys. Chem. Chem. Phys. 2000, 2, 2699] and the hydrogen bond relative strength (HBRS) criteria of Jeffrey [An Introduction to Hydrogen Bonding; Oxford University: 1997] we can provide a detailed molecular mechanism for the weakening of the intramolecular hydrogen bond based on the average dynamical structures, which clearly reveals the temperature dependence of this process. The new CPS-HBRS scheme proposed here can be utilized using any type of molecular dynamics trajectory (classical, BOMD, CPMD, etc.).

Theoretical and Experimental Investigation of Autoxidation Propensity of Selected Drugs in Solution State.

The C-H bond dissociation energy (BDE) of drug molecules is often used to estimate their relative propensities to undergo autoxidation. BDE calculations based on electronic structures provide a convenient means to estimate the risk for a given compound to degrade via autoxidation. This study aimed to verify the utility of calculated C-H BDEs of a range of drug molecules in predicting their autoxidation propensities, in the solution state. For the autoxidation study, 2,2'-azobis (2-methylpropionitrile) was employed as the solution state stressor, and the experimental reaction rate constants were determined employing ultraperformance liquid chromatographic (UPLC) methods. Reaction rates in the solution state were compared to the calculated C-H BDE values of the respective compounds. The results indicated a poor correlation for compounds in the solution state, and their relative stabilities could not be explained with C-H BDE. On the other hand, a favorable relationship was observed between the relative extent of ionization and the autoxidation rates of the selected compounds. In the solution state, factors such as the type and extent of drug ionization, degree and type of solvation have been shown to contribute to differences in reactivity. By applying the computational method involving the effect of H-atom abstraction and potential ionization sites in the molecule, the calculated C-H BDE should relate better to the experimental autoxidation rates.

Effect of degree of acidity and solvent on structural analysis of 1-(2,5-dihydroxyphenyl)-3-pyridine-2-yl-propenone and cytotoxic activity on T47D cells

Effect of degree of acidity and solvent on structural analysis of 1-(2,5-dihydroxyphenyl)-3-pyridine-2-yl-propenone and cytotoxic activity on T47D cells

Mixture design of an electrolyte system for the simultaneous separation of Cl-, SO42-, NO3-, NO2-, and HCO3- in shrimp-farming water by CZE-UV.

Shrimp is one of the most traded fishery products in the world. The shrimp-farming water ionic composition is fundamental to the growth and survival of these specimens. Therefore, this study is aimed to develop a method for the simultaneous separation of Cl-, SO42-, NO3-, NO2-, and HCO3- in this sample by capillary zone electrophoresis with UV indirect detection, without any prior sample treatment, besides dilution. The background electrolyte (BGE) was composed of CrO42- (60 mmol L-1), cetyltrimethylammonium bromide (CTAB, 2.5 mmol L-1), acetonitrile (0.875% (v/v)), and methanol (2.625% (v/v)). The mixture design optimized the BGE composition. Acetonitrile and methanol changed the degree of solvation of the anions, which decreased the radius, a phenomenon proven by calculating the radius of anions in all the conditions of the mixture design. The optimized and validated method allowed the simultaneous determination of the five above-mentioned anions in 10 min.

The influence of solvent controlled morphology on capacitive properties of metal-organic frameworks based on polyaminocarboxybenzene ligands

In order to overcome the low capacitive performance of traditional metal organic frameworks (MOFs) applied to supercapacitors, a novel conjugated small molecule monomer(3,5-diaminobenzoic acid, DABA) with amino and carboxyl groups was used as a ligand, and Ni and Co ions as metal nodes to construct novel highly electroactive bimetallic MOF(DABA-MOF) materials through a simple one-step solvothermal method. The structure and capacitive performance of obtained DABA-MOF in three organic solvents with different polarities and degrees of deprotonation (methanol, ethanol, N,N-dimethylformamide) was investigated, and it was found that with the increase of solvent deprotonation degree, the morphology of DABA-MOF with the coexistence of amino and carboxyl groups gradually changes from a smooth rod-shaped solid structure to a rough hydrangea-like structure, and the corresponding capacitive performance of DABA-MOF is also gradually enhanced. In particular, DABA-MOF synthesized in DMF can reach a maximum specific capacitance of 621 C g−1 at 1 A g−1, and the capacitance remains as high as 81.05% even after 5000 cycles, which exhibit excellent capacitance properties. This study shows that it has potential advantages to select the mixed coordination active MOF with amino and carboxyl groups as the electrode material for supercapacitor, and the deprotonation degree of solvent has a great influence on the structure and morphology of MOF with mixed active coordination sites.

Textural Characteristics of Food Confectionery Gels Using Sweeteners

Polymer gels are commonly referred to such a state of their aggregated solution, when molecular polymers chains, connected to each other by functional groups of ionic, hydrogen or dipole bonds, form a continuous solid phase, while maintaining the solvation degree (electrostatic interaction between solute and solvent particles) due to polar atomic groups remaining free for interaction. The aggregation conditions of food polymer solutions, the aggregation nature and the physico-mechanical properties of gels largely depend on the chemical polymers and solvents nature, the polymer molecules structure, technological production modes and the presence of other functional components in the food system that affect the nature and intensity of intermolecular forces. The aim of the work is to study the textural characteristics of food confectionery gels using sweeteners. The researchers developed the food confectionery gels replacing sugar with natural sweeteners, studied the textural characteristics of the confectionery gels. The study results demonstrated that sugar exclusion from the food system led to a change in the confectionery gels texture. A man can improve the textural properties of confectionery gels with the additional food composites inclusion in the gel matrix, which, in turn, will lead to an improvement not only in textural properties, but also in the nutritional value of finished products.

Self-Assembly of Colloidal Nanocrystals into 3D Binary Mesocrystals.

Biominerals are unique materials found in many living organisms that often display outstanding functionalities attributed to their mesocrystalline structure. Mesocrystals are nanocrystal superstructures with mutual crystallographic alignment of the building units. One could thus imagine these optimized evolutionary systems as archetypes to fabricate advanced materials. The main advantage of such systems relies on their ability to combine the features of the nanocrystals with those of single crystalline microscopic structures, yielding assemblies with directional, enhanced, and potentially emergent properties. Moreover, fueled by the promises of multifunctional materials with unprecedented and tunable properties, the rational design of mesocrystals assembled from two distinct colloidal nanocrystal ensembles has become a recent focus of research. However, the combination of dissimilar nanocrystals into ordered binary superstructures is still a major scientific challenge due to the nature of the coassembly process.We focus this Account on the growth of tridimensional (3D) binary mesocrystals and the understanding of the self-assembly of two colloidal nanocrystal ensembles with the ultimate goal to serve as a basis for more rational mesocrystal syntheses in the future. The formation of mesocrystals demands nanocrystals with defined surface faceting, the primary factor influencing their oriented self-assembly. Notably, such a process cannot be successfully afforded without functionalized nanocrystals with high and, in many cases, tunable colloidal stability. Besides, the nature and solvation degree of the surface ligand shell influences the effective shape of the nanocrystals and the kinetics of self-assembly. If the assembly is triggered by reducing the colloidal stability with nonsolvents, 3D single-component mesocrystals are often grown. Here, the different magnitude of the van der Waals attraction forces between nanocrystals with differing compositions, dimensions, and morphologies generally favors the segregation and growth of single component mesocrystals. This phenomenon was illustrated during the successful preparation of 3D binary mesocrystals composed of iron oxide and platinum nanocubes. Although the building blocks possessed comparable sizes and were stabilized by similar ligands, the amount of the second component could only be arbitrarily tuned up to some extent, even when the assembly conditions were rationally optimized to achieve 3D binary mesocrystals. Only a small amount of it was effectively incorporated into the matrix of the initial mesocrystal. The 3D binary mesocrystal growth process demands a delicate control over the size, shape, and surface chemistry of the nanocrystals, the solvent nature, and the self-assembly process. Hence, the improvement of our ability to control the synthesis of 3D binary mesocrystalline materials is critical to exploit their potential toward technological applications in catalysis, energy storage, or structural materials.

Dimensional Optimization for ZnO-Based Mechano-ATRP with Extraordinary Activity.

Various piezoelectric nanomaterials were utilized in ultrasound-mediated atom transfer radical polymerization (ATRP), owing to their outstanding piezoelectric effect. However, the relationship between the morphology of those piezocatalysts and polymerization has not been clearly established. Herein, we employed different piezoelectric zinc oxide (ZnO) nanomaterials to achieve novel mechano-induced ATRP (mechano-ATRP). Based on the synergistic effect of piezoelectric properties and specific surface area, the catalytic activity of 1D ZnO nanorods (1D-ZnO NRs) with increased aspect ratio outperformed that of 0D ZnO nanoparticles (0D-ZnO NPs). Compared to the conventional ATRP system, this system exhibited extraordinary activity toward the less activated monomer acrylonitrile (67% conversion after 6 h), with a narrow molecular weight distribution (polydispersity index ∼ 1.19). Furthermore, implications of ZnO loading, copper salt amount, degree of polymerization, monomer, and solvent were also studied for the highly efficient mechano-ATRP.

Combined Experimental and Computational Study of Polycyclic Aromatic Compound Aggregation: The Impact of Solvent Composition

The aggregation of polycyclic aromatic compound (PAC) molecules is sensitive to the solvent they are dissolved or suspended in. By using both dynamic light scattering and diffusion-ordered nuclear magnetic resonance spectroscopy, in combination with molecular dynamics simulations, the effect of chemical structure on the aggregation of PACs in both aromatic and alkane solvents were systematically investigated. A suite of triphenylene-based PACs offers a robust platform to understand the driving forces of aggregation mechanism across both nanometer and micrometer scales. Both the configuration, either parallel or otherwise, and the arrangement, whether compact or loose, of molecules in their aggregates are determined by a fine balance of different interactions such as those between the polar groups, π–π interactions between the aromatic cores, steric hindrance induced by the side chains, and the degree of solvation. These results suggest that molecular architecture is the major factor in determining how the model compounds aggregate. The shift from aromatic to aliphatic solvent only slightly increases the likelihood of aggregation for the model compounds studied while subtle differences in molecular architecture can have a significant impact on the aggregation characteristics.

Effect of electrolyte anions on the cycle life of a polymer electrode in aqueous batteries

Redox polymers are a class of high-capacity, low-cost electrode materials for electrochemical energy storage, but the mechanisms governing their cycling stability are not well understood. Here we investigate the effect of anions on the longevity of a p-dopable polymer through comparing two aqueous zinc-based electrolytes. Galvanostatic cycling studies reveal the polymer has better capacity retention in the presence of triflate anions than that with sulfate anions. Based on electrode microstructural analysis and evolution profiles of the cell stacking pressure, the origin of capacity decay is ascribed to mechanical fractures induced by volume change of the polymer active materials during repeated cycling. The volume change of the polymer with the triflate anion is 61% less than that with the sulfate anion, resulting in fewer cracks in the electrodes. The difference is related to the different anion solvation structures—the triflate anion has fewer solvated water molecules compared with the sulfate anion, leading to smaller volume expansion. This work highlights that anions with low solvation degree are preferable for long-term cycling.

The Influence of Sonication Processing Conditions on Electrical and Mechanical Properties of Single and Hybrid Epoxy Nanocomposites Filled with Carbon Nanoparticles.

Graphene nanoplatelets (GNP) and carbon nanotubes (CNT) are used to enhance electrical and mechanical properties of epoxy-based nanocomposites. Despite the evidence of synergetic effects in the hybrid GNP-CNT-epoxy system, there is still a lack of studies that focus on the influence of different dispersion methods on the final properties of these ternary systems. In the present work, direct and indirect ultrasonication methods were used to prepare single- and hybrid-filled GNP-CNT-epoxy nanocomposites, varying the amplitude and time of sonication in order to investigate their effect on electrical and thermomechanical properties. Impedance spectroscopy was combined with rheology and electron microscopy to show that high-power direct sonication tends to degrade electrical conductivity in GNP-CNT-epoxy nanocomposites due to damage caused in the nanoparticles. CNT-filled samples were mostly benefitted by low-power direct sonication, achieving an electrical conductivity of 1.3 × 10−3 S·m−1 at 0.25 wt.% loading, while indirect sonication was not able to properly disperse the CNTs and led to a conductivity of 1.6 ± 1.3 × 10−5. Conversely, specimens filled with 2.5 wt. % of GNP and processed by indirect sonication displayed an electrical conductivity that is up to 4 orders of magnitude higher than when processed by direct sonication, achieving 5.6 × 10−7 S·m−1. The introduction of GNP flakes improved the dispersion state and conductivity in hybrid specimens processed by indirect sonication, but at the same time impaired these properties for high-power direct sonication. It is argued that this contradictory effect is caused by a selective localization of shorter CNTs onto GNPs due to strong π-π interactions when direct sonication is used. Dynamic mechanical analysis showed that the addition of nanofillers improved epoxy’s storage modulus by up to 84%, but this property is mostly insensitive to the different processing parameters. Decrease in crosslinking degree and presence of residual solvent confirmed by Fourier-transform infrared spectroscopy, however, diminished the glass transition temperature of the nanocomposites by up to 40% when compared to the neat resin due to plasticization effects.