An official website of the United States government
AbstractElectrokinetic in-situ recovery is an alternative to conventional mining, relying on the application of an electric potential to enhance the subsurface flow of ions. Understanding the pore-scale flow and ion transport under electric potential is essential for petrophysical properties estimation and flow behavior characterization. The governing physics of electrokinetic transport is electromigration and electroosmotic flow, which depend on the electric potential gradient, mineral occurrence, domain morphology (tortuosity and porosity, grain size and distribution, etc.), and electrolyte properties (local pH distribution and lixiviant type and concentration, etc.). Herein, mineral occurrence and its associated zeta potential are investigated for EK transport. The new Ek model which is designed to solve the EK flow in complex porous media in a highly parallelizable manner includes three coupled equations: (1) Poisson equation, (2) Nernst–Planck equation, and (3) Navier–Stokes equation. These equations were solved using the lattice Boltzmann method within X-ray computed microtomography images. The proposed model is validated against COMSOL multiphysics in a two-dimensional microchannel in terms of fluid flow behavior when the electrical double layer is both resolvable and unresolvable. A more complex chalcopyrite-silica system is then obtained by micro-CT scanning to evaluate the model performance. The effects of mineral occurrence, zeta potential, and electric potential on the three-dimensional chalcopyrite-silica system were evaluated. Although the positive zeta potential of chalcopyrite can induce a flow of ferric ion counter to the direction of electromigration, the net effect is dependent on the occurrence of chalcopyrite. However, the ion flux induced by electromigration was the dominant transport mechanism, whereas advection induced by electroosmosis made a lower contribution. Overall, a pore-scale EK model is proposed for direct simulation on pore-scale images. The proposed model can be coupled with other geochemical models for full physicochemical transport simulations. Meanwhile, electrokinetic transport shows promise as a human-controllable technique because the electromigration of ions and the applied electric potential can be easily controlled externally. Graphical abstract
more »
« less
Investigation of induced electroosmotic flow in small‐scale capillary electrophoresis devices: Strategies for control and reversal
Abstract Electroosmotic flow (EOF) is the bulk flow of solution in a capillary or microchannel induced by an applied electric potential. For capillary and microchip electrophoresis, the EOF enables analysis of both cations and anions in one separation and can be varied to modify separation speed and resolution. The EOF arises from an electrical double layer at the capillary wall and is normally controlled through the pH and ionic strength of the background buffer or with the use of additives. Understanding and controlling the electrical double layer is therefore critical for maintaining acceptable repeatability during method development. Surprisingly, in fused silica capillaries at low pH, studies observe an EOF even though the capillary surface should be neutralized. Previous work has suggested the presence of an “induced electroosmotic flow” from radial electric fields generated across the capillary wall due to the separation voltage and grounded components external to the capillary. Using thin‐wall (15 µm) fused silica separation capillaries to facilitate the study of radial fields, we show that the EOF mobility depends on both the separation voltage and the location of external grounds. This is consistent with the induced EOF model, in which radial electric fields embed positive charges at the capillary walls to create an electrical double layer. The magnitude of the effect is characterized and shown to have long‐range influences that are difficult to completely null by moving grounded components away from the separation capillary. Instead, active EOF control using externally applied potentials or a passive approach using a negative separation voltage are discussed as two possible methods for controlling the induced EOF. Both methods can reverse the EOF and improve the resolution and peak efficiency in amino acid separations.
more »
« less
- Award ID(s):
- 2247387
- PAR ID:
- 10526976
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- ELECTROPHORESIS
- Volume:
- 45
- Issue:
- 19-20
- ISSN:
- 0173-0835
- Format(s):
- Medium: X Size: p. 1764-1774
- Size(s):
- p. 1764-1774
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Electroosmotic flow (EOF) has been widely used to transport fluids and samples in micro‐ and nanofluidic channels for lab‐on‐a‐chip applications. This essentially surface‐driven plug‐like flow is, however, sensitive to both the fluid and wall properties, of which any inhomogeneity may draw disturbances to the flow and even instabilities. Existing studies on EOF instabilities have been focused primarily upon Newtonian fluids though many of the chemical and biological solutions are actually non‐Newtonian. We carry out a systematic experimental investigation of the fluid rheological effects on the elastic instability in the EOF of phosphate buffer‐based polymer solutions through T‐shaped microchannels. We find that electro‐elastic instabilities can be induced in shear thinning polyacrylamide (PAA) and xanthan gum (XG) solutions if the applied direct current voltage is above a threshold value. However, no instabilities are observed in Newtonian or weakly shear thinning viscoelastic fluids including polyethylene oxide (PEO), polyvinylpyrrolidone (PVP), and hyaluronic acid (HA) solutions. We also perform a quantitative analysis of the wave parameters for the observed elasto‐elastic instabilities.more » « less
-
Abstract Backscatter interferometry (BSI) is a refractive index (RI) detection method that is easily integrated with capillary electrophoresis (CE) and is capable of detecting species ranging from inorganic ions to proteins without additional labels or contrast agents. The BSI signal changes linearly with the square of the separation voltage which has been used to quantify sample injection, but has not been explored as a potential signal enhancement mechanism in CE. Here we develop a mathematical model that predicts a signal enhancement at high field strengths, where the BSI signal is dominated by the voltage dependent mechanism. This is confirmed in both simulation and experiment, which show that the analyte peak area grows linearly with separation voltage at high field strengths. This effect can be exploited by adjusting the background electrolyte (BGE) to increase the conductivity difference between the BGE and analyte zones, which is shown to improve BSI performance. We also show that this approach has utility in small bore capillaries where larger separation fields can be applied before excess Joule heating degrades the separation. Unlike other optical detection methods that generally degrade as the optical pathlength is reduced, the BSI signal-to-noise can improve in small bore capillaries as the larger separation fields enhance the signal.more » « less
-
Abstract Dynamically controlling friction in micro- and nanoscale devices is possible using applied electrical bias between contacting surfaces, but this can also induce unwanted reactions which can affect device performance. External electric fields provide a way around this limitation by removing the need to apply bias directly between the contacting surfaces. 2D materials are promising candidates for this approach as their properties can be easily tuned by electric fields and they can be straightforwardly used as surface coatings. This work investigates the friction between single layer graphene and an atomic force microscope tip under the influence of external electric fields. While the primary effect in most systems is electrostatically controllable adhesion, graphene in contact with semiconducting tips exhibits a regime of unexpectedly enhanced and highly tunable friction. The origins of this phenomenon are discussed in the context of fundamental frictional dissipation mechanisms considering stick slip behavior, electron-phonon coupling and viscous electronic flow.more » « less
-
Abstract Sample injection in microchip‐based capillary zone electrophoresis (CZE) frequently rely on the use of electric fields which can introduce differences in the injected volume for the various analytes depending on their electrophoretic mobilities and molecular diffusivities. While such injection biases may be minimized by employing hydrodynamic flows during the injection process, this approach typically requires excellent dynamic control over the pressure gradients applied within a microfluidic network. The current article describes a microchip device that offers this needed control by generating pressure gradients on‐chip via electrokinetic means to minimize the dead volume in the system. In order to realize the desired pressure‐generation capability, an electric field was applied across two channel segments of different depths to produce a mismatch in the electroosmotic flow rate at their junction. The resulting pressure‐driven flow was then utilized to introduce sample zones into a CZE channel with minimal injection bias. The reported injection strategy allowed the introduction of narrow sample plugs with spatial standard deviations down to about 45 μm. This injection technique was later integrated to a capillary zone electrophoresis process for analyzing amino acid samples yielding separation resolutions of about 4–6 for the analyte peaks in a 3 cm long analysis channel.more » « less
