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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Dual-Ion Intercalation and High Volumetric Capacitance in a Two-Dimensional Non-Porous Coordination Polymer

Intercalation is a promising ion-sorption mechanism for enhancing the energy density of electrochemical capacitors (ECs) because it offers enhanced access to the electrochemical surface area. It requires a rapid transport of ions in and out of a host material, and it must occur without phase transformations. Materials that fulfil these requirements are rare; those that do intercalate almost exclusively cations. Herein, we show that Ni3(benzenehexathiol) (Ni 3 BHT), a non-porous two-dimensional (2D) layered coordination polymer (CP), intercalates both cations and anions with a variety of charges. Whereas cation intercalation is pseudocapacitive, anions intercalate in a purely capacitive fashion. The excellent EC performance of Ni3BHT provides a general basis for investigating similar dual-ion intercalation mechanisms in the large family of non-porous 2D CPs.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nanoarchitectonics of Metal–Organic Frameworks for Capacitive Deionization via Controlled Pyrolyzed Approaches

Abstract Next‐generation desalination technologies are needed to meet the increasing demand for clean water. Capacitive deionization (CDI) is a thermodynamically efficient technique to treat non‐potable water with relatively low salinity. The salt removal capacity and rate of CDI are highly dependent on the electrode materials, which are preferentially porous to store ions through electrosorption and/or redox reactions. Metal–organic frameworks (MOFs) with “infinite” combinations of transition metals and organic linkers simplify the production of carbonaceous materials often with redox‐active components after pyrolysis. MOFs‐derived materials show great tunability in both compositions and structures but require further refinement to improve CDI performance. This review article summarizes recent progress in derivatives of MOFs and MOF‐like materials used as CDI electrodes, focusing on the structural and compositional material considerations as well as the processing parameters and electrode architectures of the device. Furthermore, the challenges and opportunities associated with this research area are also discussed.

Wang, Hao↗
DOE OSTI2025

Dilute Regeneration-Driven Membrane Capacitive Deionization of Synthetic Seawater Using Nanopatterned Membranes and Prussian Blue Analog Electrodes

Membrane capacitive deionization (MCDI) offers energy-efficient seawater desalination but is limited at high salinity by membrane resistance and incomplete electrode regeneration. Nanopatterned ion-exchange membranes, dilute regeneration protocols, and Prussian blue analog (PBA)-functionalized electrodes are combined in a flow-by-MCDI cell. Nanopatterned ion-exchange membranes (hexagonal, octagonal, double-ring, rectangular) enhance interfacial ion transport, with hexagonal geometry delivering ≈12.5% greater surface area and the best performance. PBA-functionalized electrodes increase salt adsorption and charge-transfer kinetic rates. The integrated system lowers the area-specific resistance by 45 Ω cm2, resulting in a 500 mV reduction in the cell voltage for a current density of 2 mA cm−2 for a 35 000 ppm NaCl feed. This improves the energy-normalized salt adsorption six fold (64–382 mmol J−1). Low salinity (2000 ppm) and mixed-salt regeneration sustains a ≈39% water recovery and stable performance for at least seven cycles. Overall, combining nanopatterned membranes, which promote confinement-enhanced ion mobility, and PBA electrodes, which enhance salt adsorption, improved the energy efficiency of MCDI.

Hasan, Mahmudul↗
DOE OSTI2021

Wafer-scale quasi-layered tungstate-doped polypyrrole film with high volumetric capacitance

Layered materials are particularly attractive for supercapacitors because of their unique physical, electrical and chemical properties. In this work, we demonstrate a facile and scalable electrochemical deposition method for wafer-scale synthesis of quasi-layered tungstate-doped polypyrrole films (named TALPy) with controllable thickness and size. The as-prepared TALPy film exhibits a high gravimetric density and excellent volumetric capacitance, exceeding many high-performing carbon- and polymer-based film electrodes. Based on combined results of ex-situ X-ray diffraction (XRD), Raman and X-ray photoelectron spectroscopy (XPS), it is determined that TALPy stores charge through an ion intercalation process accompanied by change in oxidation states of polypyrrole backbone, which is referred as intercalation pseudocapacitance. All these results suggest the great promise of electrochemical deposition as a scalable and controllable bottom-up approach for synthesizing quasi-layered conductive organic-inorganic hybrid films for electrochemical energy storage applications with high volumetric performance.

36 MATERIALS SCIENCE↗
DOE OSTI2021

ESSENCE- A rapid, shear-enhanced, flow-through, capacitive electrochemical platform for rapid detection of biomolecules

The rapid, sensitive, and selective detection of target analytes using electrochemical sensors are challenging. ESSENCE, a new Electrochemical Sensor that uses a Shear-Enhanced, flowthrough Nanoporous Capacitive Electrode, overcomes current electrochemical sensors' response limitations, selectivity, and sensitivity limitations. ESSENCE is a microfluidic channel packed with transducer material sandwiched by a top and bottom microelectrode. The room-temperature instrument less integration process allows the switch of the transducer materials to make up the porous electrode without modifying the electrode architecture or device protocol. ESSENCE can be used to detect both biomolecules and small molecules by simply changing the packed transducer material. Electron microscopy results confirm the high porosity. In conjunction with the non-planar interdigitated electrode, the packed transducer material results in a flow-through porous electrode. Electron microscopy results confirm the high porosity. The enhanced shear forces and increased convective fluxes disrupt the electric double layer's (EDL) diffusive process in ESSENCE. This disruption migrates the EDL to high MHz frequency allowing the capture signal to be measured at around 100 kHz, significantly improving device timing (rapid detection) with a low signal-to-noise ratio. The device’s unique architecture allows us multiple configuration modes for measuring the impedance signal. This allows us to use highly conductive materials like carbon nanotubes. We show that by combining single-walled carbon nanotubes as transducer material with appropriate capture probes, NP-µIDE has high selectivity and sensitivity for DNA (fM sensitivity, selective against non-target DNA), breast cancer biomarker proteins (p53, pg/L sensitivity, selective against non-target HER2).

Cheng, Yu-Hsuan↗
DOE OSTI2019

Comments on “Comparison of energy consumption in desalination by capacitive deionization and reverse osmosis”

Capacitive deionization (CDI) is an emerging brackish water desalination technology in which ions are removed from water by electrostatically adsorbing them onto porous electrodes. Recently, Qin et al. presented an estimate of energy consumption for CDI schemes, and compared the energy consumption of CDI to the energy consumption of a particular reverse osmosis operation scheme which they propose. Qin et al. estimate very high values of energy consumption in CDI for brackish water desalination (e.g. ~1 to 2 g/L salt solution), and these values and trends do not agree with published experiments for CDI or with experimentally validated models for CDI. The current comment identifies important scaling errors and incorrect values in their model resistance parameters, and then discusses unphysical trends predicted by their model. We do not attempt provide a comprehensive review of their model, operation, estimates, and figures, but rather concentrate on several key issues. We present our comments in two sections dealing with resistances and energy metrics, respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Synthesis and electrochemical capacitance of long tungsten oxide nanorod arrays grown vertically on substrate

Highlights: ► Growth of long amorphous tungsten oxide nanorods on a substrate. ► Formation of single-crystalline tungsten oxide nanorods by a heat-treatment. ► High electrochemical pseudocapacitance of 2.8 mF cm{sup −2}. ► Excellent cyclability of psuedocapacitance up to 1000 cycles. -- Abstract: Long tungsten oxide nanorods are vertically grown on Al/W/Ti coated silicon substrates using a two-step anodization process. The first anodization of the Al film forms a mesh-like mask of anodic aluminum oxide, and the second anodization of the W film results in the formation of a buffer layer, a bottom nanorod, and a top nanorod of amorphous tungsten oxide. A pore-widening process prior to the second anodization leads to the enhancement of nanorod length above approximately 500 nm. After a heat-treatment, the tungsten oxide nanorods are crystallized to form a single crystalline structure while the buffer layer forms a polycrystalline structure. The crystalline tungsten oxide nanorods show a cyclic voltammogram retaining the quasi-rectangular shape of an electrochemically reversible faradaic redox reaction, i.e., a typical pseudocapacitive behavior. The maximum electrochemical capacitance per apparent surface area reaches approximately 2.8 mF cm{sup −2} at the voltage scan rate of 20 mV s{sup −1}, and the excellent cyclability of charge–discharge process is maintained up to 1000 cycles.

36 MATERIALS SCIENCE↗
DOE OSTI2014

The current–voltage and capacitance–voltage characteristics at high temperatures of Au Schottky contact to n-type GaAs

Highlights: • The electronic parameters of the diode under temperature were investigated. • The barrier heights have a Gaussian distribution. • Au/n-GaAs diode exhibits a rectification behavior. - Abstract: We have investigated the temperature-dependent current–voltage (I–V) and capacitance–voltage (C–V) characteristics of Au/n-GaAs Schottky barrier diodes (SBDs) in the temperature range of 280–415 K. The barrier height for the Au/n-type GaAs SBDs from the I–V and C–V characteristics have varied from 0.901 eV to 0.963 eV (I–V) and 1.234 eV to 0.967 eV (C–V), and the ideality factor (n) from 1.45 to 1.69 in the temperature range 280–415 K. The conventional Richardson plots are found to be linear in the temperature range measured. Both the ln(I{sub 0}/T{sup 2}) versus (kT){sup −1} and ln(I{sub 0}/T{sup 2}) versus (nkT){sup −1} plots gives a straight line corresponding to activation energies 0.773 eV and 0.870 eV, respectively. A Φ{sub b0} versus 1/T plot was drawn to obtain evidence of a Gaussian distribution of the BHs, and values of Φ{sup ¯}{sub b0} = 1.071 eV and σ{sub 0} = 0.094 V for the mean BH and zero-bias standard deviation have been obtained from this plot.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Homogeneous titanium hydroxide yields hydroxyl decorated nanofiber separator with improved electrolyte uptake and device capacitance

Good wettability of separators in batteries and capacitors is crucial for performance. Titanium hydroxide (Ti(OH) x ) has been shown to greatly improve the wettability of polyvinylidene fluoride (PVDF) nanofibers (NFs). Here, PVDF/Ti(OH) x NFs were evaluated for their potential use as separators. Results show that PVDF NFs incorporated with Ti(OH) x have improved electrolyte uptake (EU) between 550 and 1200 EU% compared to untreated PVDF with less than 100 EU%. Significant improvements in capacitance are seen from capacitors utilizing PVDF/Ti(OH) x NF separators with the best performing PVDF/Ti(OH) x NF at 15 wt% Ti(OH)x with 446.8 mF/cm 2 compared to untreated PVDF NF separator with 262.7 mF/cm 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2012

Theoretical Analysis of Effects of Deep Level, Back Contact, and Absorber Thickness on Capacitance-Voltage Profiling of CdTe Thin-Film Solar Cells

The apparent carrier density profile measured by the capacitance-voltage technique in CdTe thin-film solar cells frequently displays a distinctive U-shape. We show that, even assuming a uniform carrier density, such a U-shape may arise from deep levels, a non-ohmic back-contact, and a thin absorber, which are commonly present in practical CdTe thin-film solar cells. A thin CdTe absorber contributes to the right branch of the U-shape due to a punch-through effect at reverse or zero biases, when the CdTe absorber is nearly fully depleted. A rectifying back-contact contributes to both branches of the U-shape due to voltage sharing with the front junction under a forward bias and early punch-through under a reverse bias. Deep levels contribute to the right branch, but also raise the bottom of the U-shape, leading to an overestimate of carrier density.

14 SOLAR ENERGY↗
DOE OSTI2012

Capacitated location of collection sites in an urban waste management system

Urban waste management is becoming an increasingly complex task, absorbing a huge amount of resources, and having a major environmental impact. The design of a waste management system consists in various activities, and one of these is related to the location of waste collection sites. In this paper, we propose an integer programming model that helps decision makers in choosing the sites where to locate the unsorted waste collection bins in a residential town, as well as the capacities of the bins to be located at each collection site. This model helps in assessing tactical decisions through constraints that force each collection area to be capacitated enough to fit the expected waste to be directed to that area, while taking into account Quality of Service constraints from the citizens' point of view. Moreover, we propose an effective constructive heuristic approach whose aim is to provide a good solution quality in an extremely reduced computational time. Computational results on data related to the city of Nardo, in the south of Italy, show that both exact and heuristic approaches provide consistently better solutions than that currently implemented, resulting in a lower number of activated collection sites, and a lower number of bins to be used.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Equilibria model for pH variations and ion adsorption in capacitive deionization electrodes

Ion adsorption and equilibrium between electrolyte and microstructure of porous electrodes are at the heart of capacitive deionization (CDI) research. Surface functional groups are among the factors which fundamentally affect adsorption characteristics of the material and hence CDI system performance in general. Current CDI-based models for surface charge are mainly based on a fixed (constant) charge density, and do not treat acid-base equilibria of electrode microstructure including so-called micropores. Here, we expand current models by coupling the modified Donnan (mD) model with weak electrolyte acid-base equilibria theory. In our model, surface charge density can vary based on equilibrium constants (pK's) of individual surface groups as well as micropore and electrolyte pH environments. In this initial paper, we consider this equilibrium in the absence of Faradaic reactions. The model shows the preferential adsorption of cations versus anions to surfaces with respectively acidic or basic surface functional groups. We introduce a new parameter we term “chemical charge efficiency” to quantify efficiency of salt removal due to surface functional groups. We validate our model using well controlled titration experiments for an activated carbon cloth (ACC), and quantify initial and final pH of solution after adding the ACC sample. We also leverage inductively coupled plasma mass spectrometry (ICP-MS) and ion chromatography (IC) to quantify the final background concentrations of individual ionic species. Our results show a very good agreement between experiments and model. The model is extendable to a wide variety of porous electrode systems and CDI systems with applied potential.

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

Frequency analysis and resonant operation for efficient capacitive deionization

Capacitive deionization (CDI) performance metrics can vary widely with operating methods. Conventional CDI operating methods such as constant current and constant voltage show advantages in either energy or salt removal performance, but not both. We here develop a theory around and experimentally demonstrate a new operation for CDI that uses sinusoidal forcing voltage (or sinusoidal current). We use a dynamic system modeling approach, and quantify the frequency response (amplitude and phase) of CDI effluent concentration. Using a wide range of operating conditions, we demonstrate that CDI can be modeled as a linear time invariant system. We validate this model with experiments, and show that a sinusoid voltage operation can simultaneously achieve high salt removal and strong energy performance, thus very likely making it superior to other conventional operating methods. Based on the underlying coupled phenomena of electrical charge (and ionic) transfer with bulk advection in CDI, we derive and validate experimentally the concept of using sinusoidal voltage forcing functions to achieve resonance-type operation for CDI. Despite the complexities of the system, we find a simple relation for the resonant time scale: the resonant time period (frequency) is proportional (inversely proportional) to the geometric mean of the flow residence time and the electrical (RC) charging time. Operation at resonance implies the optimal balance between absolute amount of salt removed (in moles) and dilution (depending on the feed volume processed), thus resulting in the maximum average concentration reduction for the desalinated water. We further develop our model to generalize the resonant time-scale operation, and provide responses for square and triangular voltage waveforms as two examples. To this end, we develop a general tool that uses Fourier analysis to construct CDI effluent dynamics for arbitrary input waveforms. Using this tool, we show that most of the salt removal (~95%) for square and triangular voltage forcing waveforms is achieved by the fundamental Fourier (sinusoidal) mode. The frequency of higher Fourier modes precludes high flow efficiency for these modes, so these modes consume additional energy for minimal additional salt removed. This deficiency of higher frequency modes further highlights the advantage of DC-offset sinusoidal forcing for CDI operation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Brackish water desalination using reverse osmosis and capacitive deionization at the water-energy nexus

Here, we present a critical review of the reported performance of reverse osmosis (RO) and capacitive deionization (CDI) for brackish water (salinity < 5.0 g/L) desalination from the aspects of engineering, energy, economy and environment. We first illustrate the criteria and the key performance indicators to evaluate the performance of brackish water desalination. We then systematically summarize technological information of RO and CDI, focusing on the effect of key parameters on desalination performance, as well as energy-water efficiency, economic costs and environmental impacts (including carbon footprint). We provide in-depth discussion on the interconnectivity between desalination and energy, and the trade-off between kinetics and energetics for RO and CDI as critical factors for comparison. We also critique the results of technical-economic assessment for RO and CDI plants in the context of large-scale deployment, with focus on lifetime-oriented consideration to total costs, balance between energy efficiency and clean water production, and pretreatment/post-treatment requirements. Finally, we illustrate the challenges and opportunities for future brackish water desalination, including hybridization for energy-efficient brackish water desalination, co-removal of specific components in brackish water, and sustainable brine management with innovative utilization. Our study reveals that both RO and CDI should play important roles in water reclamation and resource recovery from brackish water, especially for inland cities or rural regions.

42 ENGINEERING↗
DOE OSTI2015

Characterization of Resistances of a Capacitive Deionization System

Capacitive deionization (CDI) is a promising desalination technology, which operates at low pressure, low temperature, requires little infrastructure, and has the potential to consume less energy for brackish water desalination. However, CDI devices consume significantly more energy than the theoretical thermodynamic minimum, and this is at least partly due to resistive power dissipation. We here report our efforts to characterize electric resistances in a CDI system, with a focus on the resistance associated with the contact between current collectors and porous electrodes. We present an equivalent circuit model to describe resistive components in a CDI cell. We propose measurable figures of merit to characterize cell resistance. We also show that contact pressure between porous electrodes and current collectors can significantly reduce contact resistance. As a result, we propose and test an alternative electrical contact configuration which uses a pore-filling conductive adhesive (silver epoxy) and achieves significant reductions in contact resistance.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Designing MOFs-Derived FeS 2 @Carbon Composites for High-Rate Sodium Ion Storage with Capacitive Contributions

We present that sodium-ion batteries suffer the disadvantages of poor rate performance and cycling stability due to its sluggish sodiation kinetics. A rational design strategy for both materials compositions and structures has been proposed to meet these challenges. Herein, a triple-component composite derived from metal organic frameworks, comprising FeS 2 , nitrogen sulfur co-doped porous carbon, and reduced graphene oxide (FeS 2 @NSC/G), has been successfully synthesized. With the capacities contributions from different sodium storage routes (diffusion-controlled processes and surface capacitive processes) at varies rate conditions, it is aiming to make full use of each component in the electrode composite and their unique porous structures. Expected electrode properties have been achieved and related electrochemical could behaviors have also been investigated. Finally, the strategy would present a promising thought for composites design, which enhance high-rate electrochemical energy storage performances.

25 ENERGY STORAGE↗
DOE OSTI2026

Pseudocapacitive Titanium Oxynitride Nanowires for Ultrahigh Capacitance Supercapacitors

High-quality, multifunctional two-dimensional (2D) titanium oxynitide (TiNO) thin films and one-dimensional (1D) TiNO nanowires have been synthesized using a pulsed laser deposition, a simple, fast, and congruent evaporation method. First-principles calculations as a function of surface orientation and termination indicate that surface oxidation of TiNO nanowires can stabilize the (110) orientation observed experimentally. The specific capacitance value for the TiNO nanowire samples (2725 mF/cm 2 ) has been found to be nearly six times more than that of the TiNO thin film samples (400 mF/cm 2 ), which is attributed to the high packing density of TiNO nanowires over a given area. The nanowire samples have also been found to exhibit a significantly higher energy density (1.35 μWh/cm 2 ) than the TiNO thin-film samples (0.33 μWh/cm 2 ). Thus, the TiNO material system in thin-film and nanowire forms has been demonstrated to be a promising candidate for use as an electrode material in supercapacitors and other charge-storage applications.

capacitors↗
DOE OSTI2019

Mapping Charge Percolation in Flowable Electrodes Used in Capacitive Deionization

Electrical percolation in flow electrode capacitive deionization is critical to mitigate electronic resistance and maximize ion electrosorption. It is experimentally challenging to characterize mass and charge transfer phenomena in flow electrodes with space and time dimensions. In this work, we demonstrate a way to resolve charge percolation pathways at sub-micron resolutions using synchrotron X-ray tomography and computational techniques. Three-dimensional reconstructed images provide a means to measure important micro- and mesoscale electrode properties, such as pore-size distribution, aggregation size, and percolation properties. Developing this microstructural understanding of flow-electrodes is necessary to understand how transport limitations impact separations performance and to inform operating conditions at the technology level (flow regimes).

36 MATERIALS SCIENCE↗