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DOE OSTI2017

Reversible Control of Interfacial Magnetism through Ionic-Liquid-Assisted Polarization Switching

The ability to control magnetism of materials via electric field enables a myriad of technological innovations in information storage, sensing, and computing. In this paper, we use ionic-liquid-assisted ferroelectric switching to demonstrate reversible modulation of interfacial magnetism in a multiferroic heterostructure composed of ferromagnetic (FM) La 0.8 Sr 0.2 MnO 3 and ferroelectric (FE) PbZr 0.2 Ti 0.8 O 3 . It is shown that ionic liquids can be used to persistently and reversibly switch a large area of a FE film. Finally, this is a prerequisite for polarized neutron reflectometry (PNR) studies that are conducted to directly probe magnetoelectric coupling of the FE polarization to the interfacial magnetization.

36 MATERIALS SCIENCE↗

DOE OSTI2021

The Influence of Water Vapor on the Electrochemical Shift of an Ionic Liquid Measured by Ambient Pressure X-ray Photoelectron Spectroscopy

Ionic liquids (ILs) are considered to be one of the steppingstones to fabricate next generation electrochemical devices given their unique physical and chemical properties. The addition of water to ILs significantly impact electrochemical related properties including viscosity, density, conductivity, and electrochemical window. Here, we utilize ambient pressure X-ray photoelectron spectroscopy (APXPS) to examine the impact of water on values of the electrochemical shift (S), which is determined by measuring changes in binding energy shifts as a function of an external bias. APXPS spectra of C 1s, O 1s and N 1s regions are examined for the IL 1-butyl-3-methylimidazolium acetate, [C 4 mim][OAc], at the IL/gas interface as a function of both water vapor pressure and external bias. Results reveal that in the absence of water vapor there is an IL ohmic drop between the working electrode and quasi reference electrode, giving rise to chemical specific S values of less than one. Upon introducing water vapor, S values approach one as a function of increasing water vapor pressure, indicating a decrease in the IL ohmic drop as the IL/water mixture becomes more conductive and the potential drop is driven by the electric double layer at the electrode/IL interface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Model for the electrical conductivity in dense plasma mixtures

A new density functional theory, average atom based model for the electrical conductivity of dense plasmas with a mixture of ion species, containing no adjustable parameters, is presented herein. The model takes the temperature, mass density and relative abundances of the species as input. It takes into account partial ionization, ionic structure, and core-valence orthogonality, and uses quantum mechanical calculations of cross sections. Comparison to an existing high fidelity but computationally expensive method reveals good agreement. The new model is computationally efficient and can reach high temperatures. A new mixing rule is also presented that gives reasonably accurate conductivities for high temperature plasma mixtures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Superior photodynamic effect of single-walled carbon nanotubes in aprotic media: a kinetic study

It has been confirmed that single-walled carbon nanotubes (SWCNTs) could generate reactive oxygen species in aprotic media by utilizing photon energy. However, the impact of photon irradiation on SWCNTs and the kinetics of the generation process in aprotic media are still unclear, which significantly limits the yield performance. In this work, the kinetics for photodynamic effects has been investigated by performing characterizations on ultraviolet-treated SWCNTs using Raman spectroscopy, conductive atomic force microscope (in-situ), kelvin probe force microscope, and X-ray photoelectron spectroscopy. It is found that ultraviolet-treated SWCNTs are observed to have more defects, lower conductivity, and less surface charge after energy conversion. Starting from the fundamental intrinsic properties of SWCNTs, the kinetics and formation of these changes are thoroughly discussed. It turns out that the dispersion, chirality, and structural integrity of SWCNTs are important for achieving high-performance photodynamic effects, which are validated using several different SWCNTs as well as other carbon nanomaterials. A type of (6,5) s-SWCNTs exhibited the highest energy efficiency among a variety of other carbon nanomaterials. The yield rate is 2.15 mM/h, and the energy consumption is determined to be 2.79 W∙h/mM. This work is expected to help dramatically boost the energy efficiency of the photodynamic effect in aprotic media and pave the way for designing high-performance carbon nanomaterial-based photoinduced devices.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Solid-state thermometry via ionic–electronic coupling in two-dimensional heterostructures

The coupling of ionic and electronic transport in solid-state systems offers new opportunities for realizing compact, energy-efficient sensing technologies, yet practical implementations remain limited. In this article, we introduce a two-dimensional iontronic platform based on field-effect transistors that integrate monolayer MoS 2 channels with van der Waals bimetallic thiophosphates ( AB P 2 X 6 , A = Li, Cu, Ag and so on; B = In, Sc and so on; and X = S and Se) as ionic gate dielectrics to realize on-chip thermometry. Specifically, we exploit thermally activated ion migration within the gate dielectric leading to conductance modulation in the MoS 2 channel for temperature sensing. We achieve ~1–2 °C resolution, fast electronic readout and subpicojoule energy consumption in an ultracompact footprint (~1 µm 2 ). Beyond thermometry, these results establish bimetallic thiophosphates as a versatile platform for solid-state iontronics and broaden the functional design space of van der Waals heterostructures for sensing, actuation and adaptive electronics.

42 ENGINEERING↗

DOE OSTI2016

Transport Properties of Ionic Liquid Mixtures Containing Heterodications

This report discusses the transport properties of ionic liquid mixtures that incorporate a series of asymmetrical dications, including heterodications. The dicationic ILs combine either triphenylphosphonium and trimethylammonium cationic sites that are bridged to methylimidazolium or methylpyrrolidinium cationic sites. Mixtures were made of the dicationic bis(trifluoromethylsulfonyl)amide ionic liquids with N-ethoxyethyl-N-methylpyrrolidinium bis(trifluoromethylsulfonyl)amide. The IL mixtures were characterized for their transport properties (temperature dependent conductivity and viscosity) and thermal properties (melting point and glass transition point).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Advances in Geophysical Monitoring Methods To Support Groundwater Remedies

Monitoring plays an important role in supporting remedial investigations and selection of remedies for groundwater contamination and for assessing performance during implementation of remedies. When a groundwater plume is near the interface between groundwater and surface water, the dynamics of groundwater flow at this interface needs to be considered in the design and implementation of a remedy. For this and other aquifer situations, groundwater flow dynamics may be difficult to evaluate through groundwater head measurements due to a sparse monitoring-well network, a relatively flat hydraulic gradient, or the presence of induced gradients from pumping operations or groundwater mounds. Geophysical approaches, coupled with other targeted measurements or the use of an ionic tracer, provide temporal data that can quantify groundwater flow dynamics. Recent developments include a flux-monitoring tool that measures fluid conductivity, bulk conductivity, and temperature at the interface between groundwater and surface water. Joint interpretation of these local data with temporal two- or three-dimensional geophysical data improves quantification of groundwater and mass flux at a targeted location. In addition, geophysical design improvements that enable the use of numerical simulations to evaluate implementation configurations and expected data resolution for geophysical methods identify threshold conditions for successful monitoring and identify the most cost-effective configurations to meet monitoring objectives.

Strickland, Christopher E.↗

DOE OSTI2019

Advances in Geophysical Monitoring Methods to Support Groundwater Remedies - 19096

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Water-mediated ion transport in an anion exchange membrane

Water is a critical component in polyelectrolyte anion exchange membranes (AEMs). It plays a central role in ion transport in electrochemical systems. Gaining a better understanding of molecular transport and conductivity in AEMs has been challenged by the lack of a general methodology capable of capturing and connecting water dynamics, water structure, and ionic transport over time and length scales ranging from those associated with individual bond vibrations and molecular reorientations to those pertaining to macroscopic AEM performance. In this work, we use two-dimensional infrared spectroscopy and semiclassical simulations to examine how water molecules are arranged into successive solvation shells, and we explain how that structure influences the dynamics of bromide ion transport processes in polynorbornene-based materials. We find that the transition to the faster transport mechanism occurs when the reorientation of water molecules in the second solvation shell is fast, allowing a robust hydrogen bond network to form. Our findings provide molecular-level insights into AEMs with inherent transport of halide ions, and help pave the way towards a comprehensive understanding of hydroxide ion transport in AEMs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2000

The Role of Electrolyte Upon the SEI Formation Characteristics and Low Temperature Performance of Lithium-Ion Cells With Graphite Anodes

Quarternary lithium-ion battery electrolyte solutions containing ester co-solvents in mixtures of carbonates have been demonstrated to have high conductivity at low temperatures (< -20C). However, in some cases the presence of such co-solvents does not directly translate into improved low temperature cell performance, presumably due to the formation of ionically resistive surface films on carbonaceous anodes. In order to understand this behavior, a number of lithium-graphite cells have been studied containing electrolytes with various ester co-solvents, including methyl acetate (MA), ethyl acetate (EA), ethyl propionate (EP), and ethyl butyrate (EB). The charge/discharge characterization of these cells indicates that the higher molecular weight esters result in electrolytes which possess superior low temperature performance in contrast to the lower molecular weight ester-containing solutions, even though these solutions display lower conductivity values.

Smart, M. C.↗

DOE OSTI2018

Ultrahigh Conductivity in Two-Dimensional InSe via Remote Doping at Room Temperature

Conductivity of two-dimenstional (2D) materials, which largely determines the efficiency and reliability of nanodevices, is proportional to the product of carrier concentration and mobility. Conventional doping, such as ionic substitution or introduction of vacancies, increases carrier concentration and decreases carrier mobility due to the scattering or trapping of carriers. In this paper, we propose a remote-doping strategy that enables the simultaneous enhancement of both parameters. Density functional theory calculations in 2D InSe reveal that adsorbing the molecule tetrathiafulvalene (TTF) and applying a 4% external tensile strain leads to an increase in the carrier concentration of the TTF-InSe system that is 13 orders of magnitude higher than that of the pristine counterpart, whereas the carrier mobility is enhanced by 35% compared with the InSe monolayer. Finally, as a consequence of the synergetic role of molecule doping and strain engineering, ultrahigh conductivity of 1.85 × 10 5 S/m is achieved in the TTF-InSe system at room temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Semiconducting High-Entropy Chalcogenide Alloys with Ambi-ionic Entropy Stabilization and Ambipolar Doping

Entropy stabilization is a novel materials-design paradigm to realize new compounds with widely tunable properties. However, almost all entropy-stabilized materials so far are either conducting metals or insulating ceramics, with a clear dearth in the semiconducting regime. Here, a new class of the multi-cationic and -anionic entropy-stabilized chalcogenide alloys based on the (Ge,Sn,Pb)(S,Se,Te) formula are synthesized and characterized experimentally. The con-figurational entropy from the disorder of both the anion and the cation sublattices reaches a record value of ~2.2 R mol -1 for the equimolar composition and stabilizes the single-phase solid solution. Theoretical calculations and experiments both show that the synthesized alloys are thermodynamically stable at the growth temperature and kinetically metastable at room temperature, segregating by spinodal decomposition at moderate temperatures. In conclusion, doping and electronic transport measurements verify that the synthesized materials are ambipolarly dopable semiconductors, which paves the way for the wider adoption of entropy-stabilized chalcogenide alloys in functional applications.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers

A series of fully fused n-type mixed conduction lactam polymers p(g 7 NC n N), systematically increasing the alkyl side chain content, are synthesized via an inexpensive, nontoxic, precious-metal-free aldol polycondensation. Employing these polymers as channel materials in organic electrochemical transistors (OECTs) affords state-of-the-art n-type performance with p(g 7 NC 10 N) recording an OECT electron mobility of 1.20 x 10 -2 cm 2 V -1 s -1 and a μC* figure of merit of 1.83 F cm -1 V -1 s -1. In parallel to high OECT performance, upon solution doping with (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)dimethylamine (N-DMBI), the highest thermoelectric performance is observed for p(g 7 NC 4 N), with a maximum electrical conductivity of 7.67 S cm -1 and a power factor of 10.4 μWm -1 K -2 . These results are among the highest reported for n-type polymers. Importantly, while this series of fused polylactam organic mixed ionic-electronic conductors (OMIECs) highlights that synthetic molecular design strategies to bolster OECT performance can be translated to also achieve high organic thermoelectric (OTE) performance, a nuanced synthetic approach must be used to optimize performance. Herein, we outline the performance metrics and provide new insights into the molecular design guidelines for the next generation of high-performance n-type materials for mixed conduction applications, presenting for the first time the results of a single polymer series within both OECT and OTE applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1981

On the significance of including the thermal motion of ions in determining the ion distribution behind a satellite

A comparative investigation concerning the spatial distribution of ions in the wake of small bodies was conducted using the theoretical wake models of Call (1969) and Parker (1976). Results for bodies with radius/ambient Debye length ratios of 2 and 5, with an electron temperature equal to the ambient electron temperature, and for the ionic Mach numbers S = 2, 4, 6, 8 are presented. Since the main physical difference between the models is in the consideration of the thermal motion of ions (Parker) versus ignoring this component (Call), a comparison between the models yields the quantitative significance of this component in determining the distribution of ions in the wake of artificial satellites. The application of this result to future experiments to be conducted on board the Spacelab and for any other large space platform in the area of space plasma physics is mentioned.

Samir, U.↗

NASA NTRS1972

Study, selection, and preparation of solid cationic conductors

Crystal chemical principles and transport theory were used to predict structures and specific compounds which might find application as solid electrolytes in rechargeable high energy and high power density batteries operating at temperatures less than 200 C. More than twenty compounds were synthesized or obtained and screened by nuclear magnetic resonance and conductivity. Many were densified by sintering or hot pressing. Encouraging results were obtained for nine of these materials but none have yet been good ionic conductors at low temperature.

Roth, W. L.↗

NASA NTRS2009

Precision Cleaning of Oxygen Systems and Components

Currently, NASA uses Dichloropentafluoropropane (HCFC-225), a Class II ozone depleting substance (ODs), to clean contaminated oxygen systems. Starting in 20 15, the Montreal Protocols and Clean Air Act prohibit the production and importation of all hydrochlorofluorocarbons (HCFC), except for limited use in refrigeration applications. Thus, a new non-ozone depleting solvent needs to be developed for use in cleaning. Optimally, such a solvent should also be environmentally benign or green to avoid needing to replace the new solvent with yet another solvent in the future due to other environmental concerns. Work for the first year consisted of two parts. The first part was developing a method of testing the cleaning efficiency of potential solvents. Stainless steel coupons were contaminated with a known weight of various contaminants and contaminant combinations and then immersed in solvent for ten minutes. The coupons were then removed and dried in an oven until all solvent had evaporated. Once dry, the coupons were weighed and the mass of the non-volatile residue (NVR) left on the coupon was determined. The cleaning efficiency of the solvents is reported as percent cleaning, with 100% cleaning being zero NVR left on the test coupon. The second half of the first goal was to use the develop method to perform baseline testing on current solvents. The second part of the work was to begin exploring alternative cleaning solvents. A variety of hydrofluorocarbons (HFCs) were tested. Preliminary testing was also performed with ionic liquids and aqueous surfactant solutions. Once potential solvents were identified, an analysis of the performance and environmental characteristics of each was to be conducted. Four contaminants were specified for use in testing. These are Mil-Spec-H-5606 (5606), a hydraulic fluid, Mil-H-83282B (83282), another hydraulic fluid, diethylhexyl sebacate (Sebacate), and WD-40. The structures of these contaminants are all similar, with long aliphatic hydrocarbon chains of lengths between fifteen and fifty. Contaminants were tested both individually and in combination. All combinations were done with equal weights of the constituent contaminants.

McLaughlin, Russell↗

DOE OSTI2018

Experimental Determination of Solubilities of Brucite [Mg(OH) 2 (cr)] in Na 2 SO 4 Solutions with Borate to High Ionic Strengths: Interactions of MgB(OH) 4 + with Na 2 SO 4

In this paper, a solubility study on brucite [Mg(OH) 2 (cr)] in Na 2 SO 4 solutions ranging from 0.01 to 1.8 mol•kg –1 , with 0.001 mol•kg –1 borate, has been conducted at 22.5°C. Based on the solubility data, the Pitzer interaction parameters for MgB(OH) 4 + —SO 4 2– and MgB(OH) 4 + —Na+ along with the formation constant for MgSO 4 (aq) are evaluated using the Pitzer model. The formation constant (log 10 β 1 0 = 2.38 ± 0.08) for MgSO 4 (aq) at 25°C and infinite dilution obtained in this study is in excellent agreement with the literature values. The experimental data on the solubility of gypsum (CaSO 4 •2H 2 O), at 25°C, in aqueous solutions of MgSO 4 with ionic strengths up to ~11 mol•kg –1 were analyzed using models with and without considering the MgSO 4 (aq) species. The model incorporating MgSO 4 (aq) fits better to the experimental data than the model without MgSO 4 (aq), especially in the ionic strength range beyond ~4 mol•kg –1 , demonstrating the need for incorporation of MgSO 4 (aq) into the model to improve the accuracy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Examination of Solvent- Room Temperature Ionic Liquid Interactions using 2D NMR and Computational Chemistry

Rare earth metals (REMs) are the key functioning material found in microelectronics, advanced batteries, and high-efficiency electrical motors. Current methods for producing REMs require high temperatures (i.e. energy intensive) and produce an abundance of hazardous fluoride waste. Room temperature ionic liquids (RTILs) are an ideal alternative electrolyte because they allow for a low-temperature, energy-efficient electrochemical process. RTIL properties such as viscosity and conductivity determine how effective they can be in this process. Since viscosity is directly related to both intra and intermolecular forces, this study sets out to investigate two RTILs-Trihexyltetradecylphosphonium dicyanamide (Cyphos 105) and Trihexyltetradecylphosphonium bistrifimide (Cyphos 109) and their interactions. Results from 2-dimensional nuclear magnetic resonance (2D NMR) spectroscopy show that there is an interaction between the tetradecyl tail and the phosphorus atom of the Cyphos RTIL. In order to establish whether this is an intra or an inter-molecular interaction, DFT-based computational calculations were performed to determine the optimized geometry. Calculations were done both in the gas phase and with propylene carbonate as an augmenting solvent. Preliminary results show that there is minimal intramolecular interaction between the tetradecyl tail and the phosphorus atom of the RTILs, and that the interaction seen in the 2D NMR experiment is likely of an intermolecular nature instead.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗