Browse
Submit Data
Databases
API
Help

Dataset Information

27 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Molecular Transport across the Ionic Liquid-Aqueous Electrolyte Interface in a MoS₂ Nanopore.

ABSTRACT: Nanopore sequencing of DNA has been enabled by the use of a biological enzyme to thread DNA through an engineered biological nanopore while recording the ionic current flowing through the nanopore. Efforts to realize a similar concept using a solid-state nanopore have been met with several technical challenges, one of which is the high speed of DNA translocation and the other the low ionic current contrast among individual nucleotides. A promising avenue to addressing both problems is using an ionic liquid to slow DNA translocation and a tiny nanopore in the MoS₂ membrane to distinguish individual nucleotides. The physical mechanisms enabling these technical advances have remained elusive. Here, we characterize the ion and DNA transport through the ionic liquid/aqueous electrolyte interface, with and without a MoS₂ nanopore, using the all-atom molecular dynamics method. We find that the partial miscibility of the ionic liquid and the aqueous electrolyte considerably alters the physics of the nanopore translocation process. Thus, the interface of the two phases generates a contact potential of 600 mV, the ionic current is dominated by the motion of ionic liquid molecules through the aqueous solution phase, and the DNA nucleotides exhibit preferential partitioning into the aqueous electrolyte, which leads to spontaneous transport of DNA polymers from the ionic liquid to the aqueous solution compartment in the absence of external voltage bias. The complex physics of the two-phase nanopore system offers a multitude of opportunities for extending the functionality of nanopore-sensing platforms.

SUBMITTER: Shankla M

PROVIDER: S-EPMC7292782 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Aqueous ionic effect on electrochemical breakdown of Si-dielectric-electrolyte interface.

Project description:The breakdown of thin dielectric films (SiO2, Si3N4, HfO2) immersed in aqueous electrolyte was investigated. The current and the kinetics of dielectric breakdown caused by large cathodic electric field applied across the dielectric layer reveal the electrochemical nature of dielectric materials. Electrolytes play a huge role in the established dielectric-electrolyte interface with respect to the overall electrical behavior of the system. Although aqueous cations are considered as spectator ions in most electrochemical systems, in dielectric interfaces the current-potential characteristics depend on the type of cation. Computer simulation based on density functional theory and molecular dynamics showed cations affect the dielectric strength. The responses of various dielectric films to solution components provide invaluable information for dielectric-incorporated electrochemical systems.

| S-EPMC7544892 | biostudies-literature

Nanoscale redox mapping at the MoS2-liquid interface.

Project description:Layered MoS2 is considered as one of the most promising two-dimensional photocatalytic materials for hydrogen evolution and water splitting; however, the electronic structure at the MoS2-liquid interface is so far insufficiently resolved. Measuring and understanding the band offset at the surfaces of MoS2 are crucial for understanding catalytic reactions and to achieve further improvements in performance. Herein, the heterogeneous charge transfer behavior of MoS2 flakes of various layer numbers and sizes is addressed with high spatial resolution in organic solutions using the ferrocene/ferrocenium (Fc/Fc+) redox pair as a probe in near-field scanning electrochemical microscopy, i.e. in close nm probe-sample proximity. Redox mapping reveals an area and layer dependent reactivity for MoS2 with a detailed insight into the local processes as band offset and confinement of the faradaic current obtained. In combination with additional characterization methods, we deduce a band alignment occurring at the liquid-solid interface.

| S-EPMC7910562 | biostudies-literature

Understanding the Electrical Transport-Structure Relationship and Photovoltaic Properties of a [Succinonitrile-Ionic Liquid]-LiI-I2 Redox Electrolyte.

Project description:The properties of succinonitrile-based electrolytes can be enhanced by the addition of an ionic liquid (IL). Here, we have reported the relationship between the electrical transport properties and the structure of a new [(1 - x)succinonitrile:xIL]-LiI-I2 electrolyte, where the mole fraction (x) of the IL (1-butyl-3-methyl imidazolium iodide) was varied from 0 to 40%. Compositional variation revealed the optimum conducting electrolyte (OCE) at x = 10 mol %, possessing an electrical conductivity (?25°C) of ?7.5 mS cm-1 with an enhancement of ?369%. The partial replacement of succinonitrile by the IL eliminated the abrupt change in the slope of the log?? vs T -1 plot at the melting temperature of the succinonitrile-LiI-I2 system, showing the Vogel-Tamman-Fulcher-type behavior owing to molecular chain disorder. Raman spectroscopy showed the I3 - concentration nearly twice the I5 - concentration for the OCE. Vibrational spectroscopy exhibited red shifts in the ?C?N, ?CH2 , ?a,CC, ?a,N-CH3 , and ?s,N-butyl modes, indicating an interaction between succinonitrile and the IL. The area ratio A CH2 /A C?N increased slightly for x = 10 mol % (OCE) and largely for x > 10 mol %, indicating an increase in the C-H bond length. These observations indicated that the interaction between succinonitrile and the IL was enhanced at x > 10 mol %, which decreased the electrical conductivity of these electrolytes. Owing to fast ion transport, an OCE-based dye-sensitized solar cell showed a 40-55% decrease in the charge-transfer and Warburg resistances, resulting in ?139 and ?122% increases in J SC and ?, respectively.

| S-EPMC7271363 | biostudies-literature

Ionic transport through a protein nanopore: a Coarse-Grained Molecular Dynamics Study.

Project description:The MARTINI coarse-grained (CG) force field is used to test the ability of CG models to simulate ionic transport through protein nanopores. The ionic conductivity of CG ions in solution was computed and compared with experimental results. Next, we studied the electrostatic behavior of a solvated CG lipid bilayer in salt solution under an external electric field. We showed this approach correctly describes the experimental conditions under a potential bias. Finally, we performed CG molecular dynamics simulations of the ionic transport through a protein nanopore (?-hemolysin) inserted in a lipid bilayer, under different electric fields, for 2-3 microseconds. The resulting I?-?V curve is qualitatively consistent with experiments, although the computed current is one order of magnitude smaller. Current saturation was observed for potential biases over ±350?mV. We also discuss the time to reach a stationary regime and the role of the protein flexibility in our CG simulations.

| S-EPMC6823379 | biostudies-literature

Thermoreversible (Ionic-Liquid-Based) Aqueous Biphasic Systems.

Project description:The ability to induce reversible phase transitions between homogeneous solutions and biphasic liquid-liquid systems, at pre-defined and suitable operating temperatures, is of crucial relevance in the design of separation processes. Ionic-liquid-based aqueous biphasic systems (IL-based ABS) have demonstrated superior performance as alternative extraction platforms, and their thermoreversible behaviour is here disclosed by the use of protic ILs. The applicability of the temperature-induced phase switching is further demonstrated with the complete extraction of two value-added proteins, achieved in a single-step. It is shown that these temperature-induced mono(bi)phasic systems are significantly more versatile than classical liquid-liquid systems which are constrained by their critical temperatures. IL-based ABS allow to work in a wide range of temperatures and compositions which can be tailored to fit the requirements of a given separation process.

| S-EPMC4740753 | biostudies-literature

A Metal-free Battery with Pure Ionic Liquid Electrolyte.

Project description:Metal or metal-ion-based batteries represent the mainstream battery technology, in which metal ions either participate in the electrode redox reaction or act as the charge carrier in the electrolyte. The principle guides battery designs and leads to the most widely adopted battery construction of metal-ion acceptor/metal salt in solvent/metal-ion donor. Although these architectures have seen significant progress, there are still many issues with them, including dendrite growth, solid-electrolyte interface corruption, and safety concerns. In this article, the intercalation/deintercalation of organic cations other than metal ions is explored in an all-organic battery composed of organic anode/cathode and pure ionic liquid electrolyte. This metal-free and solvent-free concept has been demonstrated by polyimide/1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide/polytriphenylamine full-cell, through which capacity near theoretical value, more than 5,000 cycling life, rate capability up to 200 C, and remarkable low-temperature performance has been achieved. Our work provides an alternate way of developing future efficient, safe, green, and versatile batteries.

| S-EPMC6482332 | biostudies-literature

High-Performance LiF@C-Coated FeF3·0.33H2O Lithium-Ion Batteries with an Ionic Liquid Electrolyte.

Project description:A new lithium-ion battery cathode material of LiF@C-coated FeF3·0.33H2O of 20 nm primary particles and 200-500 nm secondary particles is synthesized. The redox reaction mechanisms of the new cathode material and the influence of different electrolytes on the electrochemical performance of LiF@C-coated FeF3·0.33H2O are investigated. We show that LiF@C-coated FeF3·0.33H2O using a LiFSI/Pyr1,3 FSI ionic liquid electrolyte exhibits high reversible capacities of 330.2 and 147.6 mAh g-1 at 200 and 3600 mA g-1, respectively, as well as maintains high capacity over cycling. Electrochemical characterization shows that the high performance is attributed to higher electronic conductivity of the coating, continuous compensation of the loss of LiF product through the coating, higher ionic conductivity of both the coating and the electrolyte, and higher stability of the electrolyte.

| S-EPMC8756601 | biostudies-literature

Double-layer structure of the Pt(111)-aqueous electrolyte interface.

Project description:We present detailed measurements of the double-layer capacitance of the Pt(111)-electrolyte interface close to the potential of zero charge (PZC) in the presence of several different electrolytes consisting of anions and cations that are considered to be nonspecifically adsorbed. For low electrolyte concentrations, we show strong deviations from traditional Gouy-Chapman-Stern (GCS) behavior that appear to be independent of the nature of the electrolyte ions. Focusing on the capacitance further away from PZC and the trends for increasing ion concentration, we observe ion-specific capacitance effects that appear to be related to the size or hydration strength of the ions. We formulate a model for the structure of the electric double layer of the Pt(111)-electrolyte interface that goes significantly beyond the GCS theory. By combining two existing models, namely, one capturing the water reorganization on Pt close to the PZC and one accounting for an attractive ion-surface interaction not included in the GCS model, we can reproduce and interpret the main features the experimental capacitance of the Pt(111)-electrolyte interface. The model suggests a picture of the double layer with an increased ion concentration close to the interface as a consequence of a weak attractive ion-surface interaction, and a changing polarizability of the Pt(111)-water interface due to the potential-dependent water adsorption and orientation.

| S-EPMC8784099 | biostudies-literature

Liquid-like Poly(ionic liquid) as Electrolyte for Thermally Stable Lithium-Ion Battery.

Project description:A liquid-like poly(ionic liquid) (PIL) with a very low glass transition temperature of -51 °C and a thermal decomposition temperature of 202.7 °C was synthesized. A PIL-based electrolyte by mixing this poly(ionic liquid) with additives of 10 wt % propylene carbonate and 0.1 M LiClO4 is proved to be an excellent electrolyte for lithium-ion battery. The obtained PIL-based electrolyte exhibits a high ionic conductivity of 8.3 × 10-5 S cm-1 at 25 °C and 2.0 × 10-4 S cm-1 at 60 °C and a wide electrochemical potential window up to 5.61 V at 25 °C and 4.14 V at 60 °C. The Li/LiFePO4 batteries equipped with this PIL-based electrolyte achieve high capacity, outstanding cycling stability and rate capability at 25 °C, and even improved performance at high temperature like 60 °C. Such excellent performances of batteries are attributed to the formation of stable solid-electrolyte interface film at the lithium-electrolyte interface and the stability of electrolyte during cycling.

| S-EPMC6645412 | biostudies-literature

Modifying the Electrocatalyst–Ionomer Interface via Sulfonated Poly(ionic liquid) Block Copolymers to Enable High-Performance Polymer Electrolyte Fuel Cells

Project description: Not available

| S-EPMC10906942 | biostudies-literature