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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Harnessing Quantum Capacitance in 2D Material/Molecular Layer Junctions for Novel Electronic Device Functionality

Two-dimensional (2D) materials promise advances in electronic devices beyond Moore’s scaling law through extended functionality, such as non-monotonic dependence of device parameters on input parameters. However, the robustness and performance of effects like negative differential resistance (NDR) and anti-ambipolar behavior have been limited in scale and robustness by relying on atomic defects and complex heterojunctions. In this paper, we introduce a novel device concept that utilizes the quantum capacitance of junctions between 2D materials and molecular layers. We realized a variable capacitance 2D molecular junction (vc2Dmj) diode through the scalable integration of graphene and single layers of stearic acid. The vc2Dmj exhibits NDR with a substantial peak-to-valley ratio even at room temperature and an active negative resistance region. The origin of this unique behavior was identified through thermoelectric measurements and ab initio calculations to be a hybridization effect between graphene and the molecular layer. The enhancement of device parameters through morphology optimization highlights the potential of our approach toward new functionalities that advance the landscape of future electronics.

2D materials↗
DOE OSTI2020

Toward Water Volume Fraction Calculation in Multiphase Flows Using Electrical Capacitance Tomography Sensors

Real-time monitoring of water volume fraction in multiphase flows is an important problem for a number of industrial applications. The water phase in the multiphase flows may correspond to either the dispersed phase or the continuous phase. In the past, several lowcost and nonintrusive techniques based on the electrical capacitance tomography (ECT) has been developed to image and monitor in real-time multiphase flows containing water. Furthermore, such monitoring becomes increasingly challenging for high salinity levels, and no reliable ECTbased method is presently available which could work for obtaining water volume fraction in multiphase flows for all water salinity levels. In this paper, we propose a new approach based on the Hanai’s formula for complex dielectric constant and taking advantage of the Maxwell- Wagner-Sillars effect to obtain, to a good approximation, water volume fractions in multiphase flows containing water as either dispersed or continuous phase.

02 PETROLEUM↗
DOE OSTI2017

Flexible MXene/Graphene Films for Ultrafast Supercapacitors with Outstanding Volumetric Capacitance

A strategy to prepare flexible and conductive MXene/graphene (reduced graphene oxide, rGO) supercapacitor electrodes by using electrostatic self-assembly between positively charged rGO modified with poly(diallyldimethylammonium chloride) and negatively charged titanium carbide MXene nanosheets is presented. After electrostatic assembly, rGO nanosheets are inserted in-between MXene layers. As a result, the self-restacking of MXene nanosheets is effectively prevented, leading to a considerably increased interlayer spacing. Accelerated diffusion of electrolyte ions enables more electroactive sites to become accessible. The freestanding MXene/rGO-5 wt% electrode displays a volumetric capacitance of 1040 F cm –3 at a scan rate of 2 mV s –1 , an impressive rate capability with 61% capacitance retention at 1 V s –1 and long cycle life. Moreover, the fabricated binder-free symmetric supercapacitor shows an ultrahigh volumetric energy density of 32.6 Wh L –1 , which is among the highest values reported for carbon and MXene based materials in aqueous electrolytes. Furthermore, this work provides fundamental insight into the effect of interlayer spacing on the electrochemical performance of 2D hybrid materials and sheds light on the design of next-generation flexible, portable and highly integrated supercapacitors with high volumetric and rate performances.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Origin and tunability of unusually large surface capacitance in doped cerium oxide studied by ambient-pressure X-ray photoelectron spectroscopy

Here, the volumetric redox (chemical) capacitance of the surface of CeO 2–δ films is quantified in situ to be 100-fold larger than the bulk values under catalytically relevant conditions. Sm addition slightly lowers the surface oxygen nonstoichiometry, but effects a 10-fold enhancement in surface chemical capacitance by mitigating defect interactions, highlighting the importance of differential nonstoichiometry for catalysis.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Thermal insulation versus capacitance: A simulation experiment comparing effects of shade and hyporheic exchange on daily and seasonal stream temperature cycles

In streams where water temperatures stress native biota, management of riparian shade or hyporheic exchange are both considered viable management strategies for reducing the peaks of daily and seasonal stream channel temperature cycles. Although shade and hyporheic exchange may have similar effects on stream temperatures, their mechanisms differ. Improved understanding of the heat-exchange mechanisms influenced by shade and hyporheic exchange will aid in the appropriate application of either stream temperature management strategy. To illustrate a conceptual model highlighting shade as ‘thermal insulation’ and hyporheic exchange imparting ‘thermal capacitance’ to a stream reach, we conducted an in-silico simulation modelling experiment increasing shade or hyporheic exchange parameters on an idealized, hypothetical stream. We assessed the potential effects of increasing shade or hyporheic exchange on a stream reach using an established process-based heat-energy budget model of stream-atmosphere heat exchange and incorporated an advection-driven hyporheic heat exchange routine. The model tracked heat transport through the hyporheic zone and exchange with the stream channel, while including the effects of hyporheic water age distribution on upwelling hyporheic temperatures. Results showed that shade and hyporheic exchange similarly damped diurnal temperature cycles and differentially altered seasonal cycles of our theoretical stream. In winter, hyporheic exchange warmed simulated channel temperatures whereas shade had little effect. In summer, both shade and hyporheic exchange cooled channel temperatures, though the effects of shade were more pronounced. Our simple-to-grasp analogies of ‘thermal insulation’ for shade effects and ‘thermal capacitance’ for hyporheic exchange effects on stream temperature encourage more accurate conceptualization of complex, dynamic heat exchange processes among the atmosphere, stream channel, and alluvial aquifer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Synthesis of Microscopic 3D Graphene for High‐Performance Supercapacitors with Ultra‐High Areal Capacitance

Abstract Despite graphene being considered an ideal supercapacitor electrode material, its use in commercial devices is limited because few methods exist to produce high‐quality graphene at a large scale and low cost. A simple method is reported to synthesize 3D graphene by graphenization of coal tar pitch with a K 2 CO 3 catalyst. This produces 3D graphenes with high specific surface areas up to 2113 m 2 g −1 and exceptional crystallinity (Raman I D / I G as low as ≈0.15). The material has an outstanding specific capacitance of 182.6 F g −1 at a current density of 1.0 A g −1 . This occurs at a mass loading of 30 mg cm −2 which is 3 times higher than commercial requirements, yielding an ultra‐high areal capacitance of 5.48 F cm −2 . The K 2 CO 3 is recycled and reused over 10 cycles with material quality and electrocapacitive performance of 3D graphene retained and verified after each cycle. The synthesis method and resulting electrocapacitive performance properties create new opportunities for using 3D graphene more broadly in practical supercapacitor devices.

36 MATERIALS SCIENCE↗
DOE OSTI2019

The study of quantum efficiency in PIN photodiodes in terms of temperature and capacitive effects under non-uniform illumination conditions

In this article the impacts of quantum efficiency and bandwidth of PIN photodiodes under non-uniform illumination conditions are investigated. An absorption region is divided into the number of arbitrary layers and the continuity equations for each layer are solved with assuming that the carrier’s drift velocity is constant in each layer. Also the impact of transit time and capacitive effects of bandwidth were studied with considering the bias voltage, width of absorption region and temperature. The results show that with considering the capacitive effects, the bandwidth is increased by increase in temperature and bias voltage. We observe the effect of incident optical radiation from two n and p sides and also its impact on bandwidth and quantum efficiency. The results show more impact of radiation from n region compared to p region.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Volume Averaging Study of the Capacitive Deionization Process in Homogeneous Porous Media

Ion storage in porous electrodes is important in applications such as energy storage by supercapacitors, water purification by capacitive deionization, extraction of energy from a salinity difference and heavy ion purification. In this paper, a model is presented to simulate the charge process in homogeneous porous media comprising big pores. It is based on a theory for capacitive charging by ideally polarizable porous electrodes without faradaic reactions or specific adsorption of ions. A volume averaging technique is used to derive the averaged transport equations in the limit of thin electrical double layers. Transport between the electrolyte solution and the charged wall is described using the Gouy–Chapman–Stern model. The effective transport parameters for isotropic porous media are calculated solving the corresponding closure problems. Finally, the source terms that appear in the average equations are calculated using numerical computations. An alternative way to deal with the source terms is proposed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Modeling the Capacitive Deionization Process in Dual-Porosity Electrodes

In many areas of the world, there is a need to increase water availability. Capacitive deionization (CDI) is an electrochemical water treatment process that can be a viable alternative for treating water and for saving energy. A model is presented to simulate the CDI process in heterogeneous porous media comprising two different pore sizes. It is based on a theory for capacitive charging by ideally polarizable porous electrodes without Faradaic reactions or specific adsorption of ions. A two steps volume averaging technique is used to derive the averaged transport equations in the limit of thin electrical double layers. A one-equation model based on the principle of local equilibrium is derived. The constraints determining the range of application of the one-equation model are presented. The effective transport parameters for isotropic porous media are calculated solving the corresponding closure problems. The source terms that appear in the average equations are calculated using theoretical derivations. The global diffusivity is calculated by solving the closure problem.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2015

Graphene-containing flowable electrodes for capacitive energy storage

High conductivity and extended particle contacts are required for rapid charge percolation in flowable electrodes. In this study, carbon spheres (CS) were wrapped by highly conductive reduced graphene oxide sheets (rGO) to address these issues. We synthesized various compositions of the conductive, 3D interconnected hybrid materials (rGO@CS) using the hydrothermal method. Synergistic effects of both materials were utilized where CS served to minimize the sheet stacking for better flowability of the suspensions, and wrapped rGO sheets enabled higher conductivity for fast charge transport throughout the suspension network. When we tested as flowable electrodes, the composition with a 1:2 ratio of GO to CS exhibited the highest capacitance of 200 F/g and an improved rate performance. Moreover, the improved performance is attributed to the fast charge transport in the suspension network due to higher conductivity and enhanced connectivity of the active material particles. Optimized electrodes were also examined in a flow mode which yielded a capacitance of 45 F/g.

36 MATERIALS SCIENCE↗
DOE OSTI2015

High rate capacitive performance of single-walled carbon nanotube aerogels

Single-walled carbon nanotube (SWCNT) aerogels produced by critical-point-drying of wet-gel precursors exhibit unique properties, such as high surface-area-to-volume and strength-to-weight ratios. They are free-standing, are binder-free, and can be scaled to thicknesses of more than 1 mm. In this paper, we examine the electric double layer capacitive behavior of these materials using a common room temperature ionic liquid electrolyte, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMI-TFSI). Electrochemical performance is assessed through galvanostatic cycling, cyclic voltammetry and impedance spectroscopy. Results indicate stable capacitive performance over 10,000 cycles as well as an impressive performance at high charge and discharge rates, due to accessible pore networks and enhanced electronic and ionic conductivities of SWCNT aerogels. Finally, these materials can find applications in mechanically compressible and flexible supercapacitor devices with high power requirements.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Engineered MXene quantum dots for micro-supercapacitors with excellent capacitive behaviors

Micro-supercapacitors (MSCs) have drawn tremendous attention as promising candidates to power miniaturized portable/wearable electronics, but they still suffer from unsatisfactory electrochemical performance (e.g., insufficient energy density, mediocre rate capability), thus impeding their widespread applications. Here, a synergistic surface and structure engineering strategy achieved by downsizing to quantum dot scale, doping of heteroatoms, and introducing defects and functional groups is proposed to regulate the physicochemical properties of Ti 3 C 2 T x MXene. Encouragingly, the resulting MSCs based on defect-rich nitrogen-doped Ti 3 C 2 T x quantum dots (QDs) possess excellent electrochemical performance as demonstrated by large operating voltage (3.0 V in ionic liquid and 1.0 V in aqueous electrolyte), perfect rectangular CV shape even at 1000 V·s -1 , high volumetric capacitance of 33.1 F·cm -3 , and superior cycling stability after 10000 cycles. By employing experimental characterizations and density functional theory calculations, the remarkable performance of the MSCs is mainly due to the special chemical states as well as the unique surface and structural features of Ti 3 C 2 T x QDs, which offer abundant active sites, shorten ion diffusion pathways, promote ion/electron transports, and provide enhanced capacitance. Finally, this work provides a new strategy for the design of high-performance MSCs and a reference for the applications of MXene QDs in other energy-related fields.

42 ENGINEERING↗
DOE OSTI2020

The Development of a Generalized Riser Flow Regime Map Based Upon Higher Moment and Chaotic Statistics Using Electrical Capacitance Volume Tomography (ECVT)

Dynamic analyses have been applied to the temporal signals from an Electro Capacitance Volume Tomography instrument located near mid-height on the riser of an industrial-scale cold-flow circulating fluidized bed to characterize gas-solids flow behavior in the riser. Twelve capacitance electrodes surround the cylindrical riser over a height of 1.3 m. The instrument used a neural network deconvolution algorithm to determine the spatially resolved solids fraction recorded at 52 Hz. Experiments were carried out over a range of gas and solids flows in the transport regime using a Geldart Group B bed material, high density polyethylene with mean particle size of 880 μm. The radial solids distribution was found to vary from one-time step to the next between profiles typical of laminar and turbulent flow. The duration of time spent in each of these flow profiles depended upon the operating regime – dilute, core-annular, or fast fluidized bed. The chaotic structure of the temporal data was characterized using the three conventional approaches: the first 4 moments from the distribution of signal in time, system memory parameters from the autocorrelation function and the Hurst exponent, and analysis of the correlationentropy and correlation dimension of the attractor. These signal analysis techniques were used to clearly distinguish differences between different transport operating regimes. Specifically, it was experimentally observed that a riser transitions from core annular flow profile to dilute and dense regimes via increasing the frequency of short term transients to either dilute or dense flow profiles, respectively. A regime map was generated based upon these dynamics using solids flux and gas velocity axes. Fast fluidized, core annular, and dilute each exhibited different degree of dynamic characteristics typical of fluid dominated or particle compromising behavior. It should be noted that the magnitude for the different statistics was in the same range regardless of the regime, it was the radial profile for the statistic that changed and subsequently identified that there was a change in the regime. Finally, a reduced regime map was developed consisting of plotting the gas velocity normalized by the upper transport velocity versus the solids flux normalized by the saturation carrying capacity. The use of this reduced plot allowed the data from widely different conditions to be plotted and compared on the same<p>graph. Note that in many instances, some of the statistics identified the operating point as being in one regime while others indicated that it was in another indicating a transition region between dilute or core annular regimes and between the core annular and fast fluidization regimes. This now provides a tool that can be used to optimize process performance, identify changes in operating states, or replicate process dynamics during process scaling or changing operating parameters. </p>

Breault, Ronald↗
DOE OSTI2018

Self similarities in desalination dynamics and performance using capacitive deionization

Charge transfer and mass transport are two underlying mechanisms which are coupled in desalination dynamics using capacitive deionization (CDI). We developed simple reduced-order models based on a mixed reactor volume principle which capture the coupled dynamics of CDI operation using closed-form semi-analytical and analytical solutions. We use the models to identify and explore self-similarities in the dynamics among flow rate, current, and voltage for CDI cell operation including both charging and discharging cycles. The similarity approach identifies the specific combination of cell (e.g. capacitance, resistance) and operational parameters (e.g. flow rate, current) which determine a unique effluent dynamic response. We here demonstrate self-similarity using a conventional flow between CDI (fbCDI) architecture, and we hypothesize that our similarity approach has potential application to a wide range of designs. We performed an experimental study of these dynamics and used well-controlled experiments of CDI cell operation to validate and explore limits of the model. For experiments, we used a CDI cell with five electrode pairs and a standard flow between (electrodes) architecture. Guided by the model, we performed a series of experiments that demonstrate natural response of the CDI system. We also identify cell parameters and operation conditions which lead to self-similar dynamics under a constant current forcing function and perform a series of experiments by varying flowrate, currents, and voltage thresholds to demonstrate self-similarity. Based on this study, we hypothesize that the average differential electric double layer (EDL) efficiency (a measure of ion adsorption rate to EDL charging rate) is mainly dependent on user-defined voltage thresholds, whereas flow efficiency (measure of how well desalinated water is recovered from inside the cell) depends on cell volumes flowed during charging, which is determined by flowrate, current and voltage thresholds. Results of experiments strongly support this hypothesis. Results show that cycle efficiency and salt removal for a given flowrate and current are maximum when average EDL and flow efficiencies are approximately equal. We further explored a range of CC operations with varying flowrates, currents, and voltage thresholds using our similarity variables to highlight trade-offs among salt removal, energy, and throughput performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Ion selectivity in capacitive deionization with functionalized electrode: Theory and experimental validation

Capacitive deionization (CDI) is a promising technique for salt removal and may have potential for highly selective removal of ion species. In this work, we take advantage of functional groups usually used with ionic exchange resins and apply these to CDI. To this end, we functionalize activated carbon with a quaternary amines surfactant and use this surface to selectively and passively (no applied field) trap nitrate ions. We then set the cell voltage to a constant value to regenerate these electrodes, resulting in an inverted capacitive deionization (i-CDI) operation. Unlike resins, we avoid use of concentrated chemicals for regeneration. We measure the selectivity of nitrate versus chloride ions as a function of regeneration voltage and initial chloride concentration. We experimentally demonstrate up to about 6.5-fold (observable) selectivity in a cycle with a regeneration voltage of 0.4 V. We also demonstrate a novel multi-pass, air-flush i-CDI operation to selectively enrich nitrate with high water recovery. We further present a dynamic, multi-species electrosorption and equilibrium solution-to-surface chemical reaction model and validate the model with detailed measurements. Our i-CDI system exhibits higher nitrate selectivity at lower voltages; making it possible to reduce NaNO 3 concentrations from ~170 ppm to below the limit of maximum allowed values for nitrate in drinking water of about 50 ppm NaNO 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Using Ultramicroporous Carbon for the Selective Removal of Nitrate with Capacitive Deionization

The contamination of water resources with nitrate is a growing and significant problem. Here we report the use of ultramicroporous carbon as a capacitive deionization (CDI) electrode for selectively removing nitrate from an anion mixture. Through moderate activation, we achieve a micropore-size distribution consisting almost exclusively of narrow (<1 nm) pores that are well suited for adsorbing the planar, weakly hydrated nitrate molecule. Cyclic voltammetry measurements reveal an enhanced capacitance for nitrate when compared to chloride as well as significant ion sieving effects when sulfate is the only anion present. We measure high selectivities ( S ) of both nitrate over sulfate ( S NO 3 /SO 4 = 17.8 ± 3.6 at 0.6 V) and nitrate over chloride ( S NO 3 /Cl = 6.1 ± 0.4 at 0.6 V) when performing a constant voltage CDI separation on 3.33 mM/3.33 mM/1.67 mM Cl/NO 3 /SO 4 feedwater. Furthermore, these results are particularly encouraging considering that a divalent interferant was present in the feed. Using molecular dynamics simulations, we examine the solvation characteristics of these ions to better understand why nitrate is preferentially electrosorbed over sulfate and chloride.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Two-Dimensional Porous Electrode Model for Capacitive Deionization

Here, ion transport in porous conductive materials is of great importance in a variety of electrochemical systems including batteries and supercapacitors. We here analyze the coupling of flow and charge transport and charge capacitance in capacitive deionization (CDI). In CDI, a pair of porous carbon electrodes is employed to electrostatically retain and remove ionic species from aqueous solutions. We here develop and solve a novel unsteady two-dimensional model for capturing the ion adsorption/desorption dynamics in a flow-between CDI system. We use this model to study the complex, nonlinear coupling between electromigration, diffusion, and advection of ions. We also fabricated a laboratory-scale CDI cell which we use to measure the near-equilibrium, cumulative adsorbed salt, and electric charge as a function of applied external voltage. We use these integral measures to validate and calibrate this model. We further present a detailed computational study of the spatiotemporal adsorption/desorption dynamics under constant voltage and constant flow conditions. We show results for low (20 mM KCl) and relatively high (200 mM KCl) inlet ion concentrations and identify effects of ion starvation on desalination. We show that in both cases electromigrative transport eventually becomes negligible and diffusive ion transport reduces the desalination rate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Ionic Liquid Mixture Expands the Potential Window and Capacitance of a Supercapacitor in Tandem

Mixing room temperature ionic liquids (RTIL) may optimize electrolyte properties for the better performance of electrical double layer capacitors (EDLCs). To understand the composition effects, we theoretically investigate the potential window, interfacial structure, capacitance, and energy density of RTIL mixtures consisting of one common cation and two anions of different sizes. A combination of quantum density functional theory (QDFT) and classical density functional theory (CDFT) calculations indicates that the electrolyte composition has significant effects on the EDL structure and potential of zero charge, thereby altering the integral capacitance and electrochemical potential window. The two quantities can be optimized together to achieve the best EDLC performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗