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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 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Accelerated Characterization of Electrode‐Electrolyte Equilibration

Operational durability is poorly characterized by traditional (photo)electrocatalyst discovery workflows, creating a barrier to scale-up and deployment. Corrosion is a prominent degradation mechanism whose thermodynamics depend on the concentration of corrosion products in electrolyte. We present an automated system for characterizing the equilibration of (photo)electrodes with dissolved metals in electrolyte for a given electrode, pH, and electrochemical potential. Automation of electrode selection, electrolyte preparation, and electrolyte aliquoting enables rapid identification of self-passivating electrodes and estimation of the equilibrium dissolved metals concentrations. The technique is demonstrated for metal oxide photoanodes in alkaline electrolyte, where BiVO 4 is found to continually corrode, in agreement the literature. An amorphous Ni−Sb−O photoanode is found to passivate with a Ni-rich coating on the order of 1 monolayer with less than 1 μM total dissolved metals in electrolyte, demonstrating its suitability for durable photoelectrochemical operation. The automation and throughput of the instrument are designed for incorporation in accelerated electrocatalyst discovery workflows so that durability can be considered on equal footing with activity.

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

Sustainable Direct Recycling of Lithium-Ion Batteries via Solvent Recovery of Electrode Materials

Separation of electrode materials from their current collectors is an enabling step toward recovering critical materials from spent lithium-ion batteries. In this study, a highly efficient, cost-effective, and environmentally sustainable separation process was developed for that purpose. Ethylene glycol, a vital commodity chemical as an antifreeze and polymer precursor, is used to delaminate electrode materials at low temperatures in seconds without altering the crystalline structure and morphology of active electrode materials. The recovered current collectors were intact without any corrosion. The authors also found that the solvent could be continuously reused, leading to the development of a closed-loop ecosystem and lithium-ion battery circular economy. The ultrafast delamination was driven by the competitive inhibition of binding through the weakening of hydrogen bonding. The ethylene glycol-based separation is a sustainable electrode recovery process that paves the way for battery recycling.

25 ENERGY STORAGE↗
DOE OSTI2021

Switching CO 2 Electroreduction Selectivity Between C 1 and C 2 Hydrocarbons on Cu Gas-Diffusion Electrodes

We report that regulating the selectivity toward a target hydrocarbon product is still the focus of CO 2 electroreduction. Here, we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important role than the surface roughness, local pH, and facet in governing the selectivity toward C 1 or C 2 hydrocarbons. The selectivity toward C 2 H 4 progressively increases, while CH 4 decreases steadily upon lowering the Cu oxidation species fraction. At a relatively low electrodeposition voltage of 1.5 V, the Cu gas-diffusion electrode with the highest Cu δ+ /Cu 0 ratio favors the pathways of hydrogenation to form CH 4 with maximum Faradaic efficiency of 65.4% and partial current density of 228 mA cm -2 at -0.83 V vs RHE. At 2.0 V, the Cu gas-diffusion electrode with the lowest Cu δ+ /Cu 0 ratio prefers C–C coupling to form C 2+ products with Faradaic efficiency topping 80.1% at -0.75 V vs RHE, where the Faradaic efficiency of C 2 H 4 accounts for 46.4% and the partial current density of C 2 H 4 achieves 279 mA cm -2 . This work demonstrates that the selectivity from CH 4 to C 2 H 4 is switchable by tuning surface Cu species composition of Cu gas-diffusion electrodes.

36 MATERIALS SCIENCE↗
DOE OSTI2021

High Energy Density and Stable Three-Dimensionally Structured Se-Loaded Bicontinuous Porous Carbon Battery Electrodes

Here, 3D structured Se-loaded bicontinuous porous carbon (BPC) electrodes were fabricated through colloidal templating of BPC followed by pulsed-voltage Se electrodeposition. The resultant electrodes were found to deliver a specific capacity of 665 mA h g -1 at a rate of 0.1 C, near the theoretical value for Se. When a vinylene carbonate containing electrolyte was utilized, the capacity fade over 500 cycles at 1 C rate was as small as a few percent. Impedance measurements and physical characterization of cycled electrodes indicated the exceptionally stable cycling performance was possibly due to vinylene carbonate resulting in formation of a stable SEI during cycling. Along with cycling stability, the rate performance of the 3D Se/BPC electrodes was also good. Due to the bicontinuous structure of carbonaceous current collector at rates as high as 5 C, the deliverable capacity was about 300 mA h g -1 .

25 ENERGY STORAGE↗
DOE OSTI2020

Electrowetting‐Mediated Transport to Produce Electrochemical Transistor Action in Nanopore Electrode Arrays

Abstract Understanding water behavior in confined volumes is important in applications ranging from water purification to healthcare devices. Especially relevant are wetting and dewetting phenomena which can be switched by external stimuli, such as light and electric fields. Here, these behaviors are exploited for electrochemical processing by voltage‐directed ion transport in nanochannels contained within nanopore arrays in which each nanopore presents three electrodes. The top and middle electrodes (TE and ME) are in direct contact with the nanopore volume, but the bottom electrode (BE) is buried beneath a 70 nm silicon nitride (SiN x ) insulating layer. Electrochemical transistor operation is realized when small, defect‐mediated channels are opened in the SiN x . These defect channels exhibit voltage‐driven wetting that mediates the mass transport of redox species to/from the BE. When BE is held at a potential maintaining the defect channels in the wetted state, setting the potential of ME at either positive or negative overpotential results in strong electrochemical rectification with rectification factors up to 440. By directing the voltage‐induced electrowetting of defect channels, these three‐electrode nanopore structures can achieve precise gating and ion/molecule separation, and, as such, may be useful for applications such as water purification and drug delivery.

Kwon, Seung‐Ryong↗
DOE OSTI2022

Latticed-Confined Conversion Chemistry of Battery Electrode

The electrochemical conversion reaction, usually featured by multiple redox processes and high specific capacity, holds great promise in developing high energy rechargeable battery technologies. However, the complete structural change accompanied by spontaneous atomic migration and volume variation during the charge/discharge cycle leads to electrode disintegration and performance degradation, therefore severely restricting the application of conventional conversion-type electrodes. Herein, latticed-confined conversion chemistry is proposed, where the “intercalation-like” redox behavior is realized on the electrode with a “conversion-like” high capacity. By delicately formulating the high-entropy compounds, the pristine crystal structure can be preserved by the inert lattice framework, thus enabling an ultra-high initial Coulombic efficiency of 92.5% and a long cycling lifespan over a thousand cycles after the quasistatic charge–discharge cycle. This lattice-confined conversion chemistry unfolds a ubiquitous insight into the localized redox reaction and sheds light on developing high-performance electrodes toward next-generation high-energy rechargeable batteries.

25 ENERGY STORAGE↗
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

Chemical Heterointerface Engineering on Hybrid Electrode Materials for Electrochemical Energy Storage

Abstract The chemical heterointerfaces in hybrid electrode materials play an important role in overcoming the intrinsic drawbacks of individual materials and thus expedite the in‐depth development of electrochemical energy storage. Benefiting from the three enhancement effects of accelerating charge transport, increasing the number of storage sites, and reinforcing structural stability, the chemical heterointerfaces have attracted extensive interest and the electrochemical performances of hybrid electrode materials have been significantly optimized. In this review, recent advances regarding chemical heterointerface engineering in hybrid electrode materials are systematically summarized. Especially, the intrinsic behaviors of chemical heterointerfaces on hybrid electrode materials are refined based on built‐in electric field, van der Waals interaction, lattice mismatch and connection, electron cloud bias and chemical bond, and their combination. The strategies for introducing chemical heterointerfaces are classified into in situ local transformation, in situ growth, cosynthesis, and other strategy. The recent progress about the chemical heterointerfaces engineering specially focusing on metal‐ion batteries, supercapacitors, and Li–S batteries are introduced in detail. Furthermore, the classification and characterization of chemical heterointerfaces are briefly described. Finally, the emerging challenges and perspectives about future directions of chemical heterointerface engineering are proposed.

Li, Wenbin↗
DOE OSTI2021

Perovskite Photovoltaic Devices with Carbon-Based Electrodes Withstanding Reverse-Bias Voltages up to –9 V and Surpassing IEC 61215:2016 International Standard

One of the key challenges of perovskite photovoltaics (PV) is the long-term stability. Although efforts are made to improve the lifetime of perovskite PV devices, their degradation under reverse-bias conditions is barely addressed. Herein, perovskite solar cells with carbon-based electrodes are presented which demonstrate superior resilience against reverse-bias-induced degradation. Although their breakdown voltage is identified to be at approximately -3.6 V, cells do not degrade until the applied reverse-bias exceeds -9 V. Two main degradation mechanisms are identified: 1) iodine loss due to hole tunneling into perovskite, which takes place even at low reverse-bias but decomposes the perovskite only after long time durations; and 2) rapid heating at large reverse-bias leading to formation of PbI2, which starts at shunts and then follows the path of the least resistance for the cell current, which is primarily influenced by the electrode sheet resistances. Finally, perovskite solar modules with carbon-based electrodes are demonstrated, which are subjected to a "hotspot" test described in the IEC 61215:2016 international standard at an accredited module testing laboratory. Passing this accelerated test for the first time confirms the superior stability of perovskite PV devices with carbon-based electrodes and highlights their large industrialization potential.

14 SOLAR ENERGY↗
DOE OSTI2024

Topology optimization for the full-cell design of porous electrodes in electrochemical energy storage devices

In this paper, we introduce a density-based topology optimization framework to design porous electrodes for maximum energy storage. We simulate the full cell with a model that incorporates electronic potential, ionic potential, and electrolyte concentration. The system consists of three materials, namely pure liquid electrolyte and the porous solids of the anode and cathode, for which we determine the optimal placement. We use separate electronic potentials to model each electrode, which allows interdigitated designs. As a result, a penalization is required to ensure that the anode and cathode do not touch, i.e., causing a short circuit. We compare multiple 2D designs generated for different fixed conditions, e.g. material properties. A 3D design with complex channel and interlocked structure is also created. All optimized designs are far superior to the traditional monolithic electrode design with respect to energy storage metrics. We observe up to a 750% increase in energy storage for cases with slow effective ionic diffusion within the porous electrode.

25 ENERGY STORAGE↗
DOE OSTI2022

Role of nanocellulose in tailoring electroanalytical performance of hybrid nanocellulose/multiwalled carbon nanotube electrodes

Abstract Nanocellulose has emerged as a promising green dispersant for carbon nanotubes (CNTs), and there is an increasing trend in developing nanocellulose/CNT hybrid materials for electrochemical detection of various small molecules. However, there have been very few comprehensive studies investigating the role of nanocellulosic material properties upon the electroanalytical performance of the resultant hybrid electrodes. In this work, we demonstrate the influence of both nanocellulose functionalization and geometry, utilizing sulfated cellulose nanocrystals, sulfated cellulose nanofibers, and TEMPO-oxidized cellulose nanofibers. Transmission electron microscopy tomography enables direct visualization of the effect of nanocellulosic materials on the hybrid architectures. High resolution X-ray absorption spectroscopy verifies that the chemical nature of CNTs in the different hybrids is unmodified. Electroanalytical performances of the different nanocellulose/CNT hybrid electrodes are critically evaluated using physiologically relevant biomolecules with different charge such as, dopamine (cationic), paracetamol (neutral), and uric acid (anionic). The hybrid electrode containing fibrillar nanocellulose geometry with a high degree of sulfate group functionalization provides the highest electroanalytical sensitivity and strongest enrichment towards all studied analytes. These results clearly demonstrate for the first time, the extent of tailorability upon the electroanalytical response of nanocellulose/CNT hybrid electrodes towards different biomolecules, offered simply by the choice of nanocellulosic materials.

Durairaj, Vasuki↗
DOE OSTI2022

Scalable membrane-less microbial electrolysis cell with multiple compact electrode assemblies for high performance hydrogen production

Bioelectrochemical hydrogen production via microbial electrolysis cells (MECs) is a promising method for sustainable energy production and decarbonization of energy systems. However, the application of MECs is limited by the electrochemical performance, scalability, and the cost associated with expensive materials. Here, in this study, a scalable MEC (500 mL) with novel compact electrode assemblies and high electrode surface area to volume ratio (160 m 2 /m 3 ) was designed and constructed. The use of membranes, precious metal catalyst, and current collectors with high costs was avoided. A high current density at the steady state of 49.5 ± 5.3 A/m 2 was achieved using acetate as the substrate with phosphate buffer under the applied voltage of 1.01 V. The corresponding volumetric current density was 3948 ± 422 A/m 3 . The compact electrode assembly design limited methane production rate to 3.9 ± 0.2 L/L/D, while achieving a hydrogen production rate of 33.7 ± 1.7 L/L/D. With the suppression of microbial hydrogen consumption, the hydrogen production rate was 39.8 ± 1.9 L/L/D, higher by almost one order of magnitude than those of MECs with scaling up attempts. The compact electrode configuration reduced internal resistance to 88.5 ± 4.4 Ω cm 2 . The energy efficiency based on input electricity was 146 ± 7 % to 189 ± 9 % within the applied voltage range of 0.71 to 1.05 V. The results in this study demonstrated successful scaling up of high performance small MECs and offered a new possible approach of scaling up MECs by stacking high-performance subunits, with no trade-offs on electrochemical performance.

08 HYDROGEN↗
DOE OSTI2021

Insight on electrolyte infiltration of lithium ion battery electrodes by means of a new three-dimensional-resolved lattice Boltzmann model

Electrolyte filling takes place between sealing and formation in Lithium Ion Battery (LIB) manufacturing process. This step is crucial as it is directly linked to LIB quality and affects the subsequent time consuming electrolyte wetting process. Although having fast, homogeneous and complete wetting is of paramount importance, this process has not been sufficiently examined and fully understood. For instance, experimentally available data is insufficient to fully capture the complex interplay upon filling between electrolyte and air inside the porous electrode. We report here for the first time a 3D-resolved Lattice Boltzmann Method (LBM) model able to simulate electrolyte filling upon applied pressure of LIB porous electrodes obtained both from experiments (micro X-ray tomography) and computations (stochastic generation, simulation of the manufacturing process using Coarse Grained Molecular Dynamics and Discrete Element Method). The model allows obtaining advanced insights about the impact of the electrode mesostructures on the speed of electrolyte impregnation and wetting, highlighting the importance of porosity, pore size distribution and pores interconnectivity on the filling dynamics. Furthermore, we identify scenarios where volumes with trapped air (dead zones) appear and evaluate the impact of those on the electrochemical behavior of the electrodes.

25 ENERGY STORAGE↗
DOE OSTI2021

An ultrathin solid-state electrolyte film coated on LiNi 0.8 Co 0.1 Mn 0.1 O 2 electrode surface for enhanced performance of lithium-ion batteries

We report layered Ni-rich oxide is a promising cathode material for lithium-ion batteries (LIBs) of high energy density, yet its poor electrochemical stability induced by electrode-electrolyte interfacial degradation has still needed to be addressed. Surface coating is one of the powerful techniques to tackle this issue, nevertheless, it has been extensively used on particle but not electrode regarding a larger area of protection. Herein, we have covered a nano-scaled layer of lithium phosphorus oxynitride (LiPON) on the electrode level of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM) surface and found lower impedance, longer cycle life, and better safety for treated battery. Most notably, such an NCM-LiPON based 1.3 Ah pouch cell delivers an energy density of 364.4 Wh kg -1 (based on positive and negative materials), along with the retention of 80.0% over 745 cycles at 0.5 C-rate, which is 1.3 times longer than the bare one. This results from modification of both superficial cathode-electrolyte interphase (CEI) and structure stabilization of general particle surface, therefore, role of conformal coating upon electrode surface should be highlighted.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Design and processing for high performance Li ion battery electrodes with double-layer structure

A two-layer LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode has been designed and fabricated containing a “power layer” and “energy layer”, with corresponding porosity and particle size prescribed to each layer to achieve best utilization of electrode material (maximum integrated depth of discharge across the electrode thickness) at high applied current. The cathode showed a 17% improvement in capacity when tested in symmetric cells. When applying the design to a full cell, where both positive and negative electrodes contain power and energy layers, a 74% increase in discharge capacity at 2C was achieved compared to the cell with conventional electrodes. Furthermore, this demonstrates an avenue to increase energy and power density of lithium–ion batteries and enable fast charging capability.

25 ENERGY STORAGE↗
DOE OSTI2024

Direct reuse of graphite and lithium nickel manganese cobalt oxide (NMC) recovered from ultrafast-laser ablation debris in Li-ion battery electrodes

Here we demonstrate that debris collected from the ultrafast-laser ablation of graphite anodes can be directly reused in a lithium-ion battery with little to no negative effects on electrochemical performance. Further, we show that while post-ablation NMC (LiNi 0.33 Mn 0.33 Co 0.33 O) cathode debris will require additional processing before being incorporated into an electrode, its critical materials (nickel, manganese, and cobalt) are not lost during ablation and can be recovered for recycling. Pre- and post-ablation materials are characterized with a suite of diagnostics, including SEM, TEM, X-ray CT, EDS, and XRD, to study changes in material morphology, composition and crystal structure. Graphite exhibited little to no morphological or compositional changes and a slight annealing of its crystal structure. NMC underwent profound morphological and crystallographic changes, but retained its elemental composition. Finally, post-ablation materials were re-manufactured into electrodes and cycled vs lithium metal. Graphite showed equal or better capacity and Coulombic efficiency compared to pre-ablation electrodes, while the post-ablation NMC exhibited severely reduced electrochemical performance. Furthermore, we discuss the outlook for application of this work to advanced manufacturing lines that produce next-generation, laser-patterned electrodes.

25 ENERGY STORAGE↗
DOE OSTI2025

Surface modification of cathode material enhances electrochemical performance in dry-processed Li-ion battery electrodes

The transition to electric vehicles (EVs) is pivotal for achieving energy security and integrating grid stability, with lithium-ion batteries (LIBs) playing a central role in this transformation. However, the conventional wet electrode manufacturing relying on N-methyl-2-pyrrolidone (NMP) solvent is energy intensive and costly. Dry processing (DP) has emerged as a promising alternative, eliminating solvents and using polytetrafluoroethylene (PTFE) binder for electrode fabrications. Despite its advantages, DP faces a critical challenge: poor interfacial adhesion between the hydrophobic PTFE binder and the hydrophilic cathode active material (CAM), particularly LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811), which undermines electrode performance. Here, to address this, we introduced a novel vapor-phase trimethoxymethylsilane (TMMS) coating to hydrophobize the CAM surface, enhancing compatibility with PTFE. This surface modification significantly enhances binder – CAM interactions, enabling uniform mixing and robust electrode integrity without damaging the CAM particles. Our findings advance the feasibility of environmentally sustainable and cost-effective dry processing, representing a significant step toward sustainable battery manufacturing.

Choi, Junbin [Oak Ridge National Laboratory (ORNL)↗
DOE OSTI2023

Development and Characterization of Electrodes for Surface-Specific Attenuated Total Reflection Two-Dimensional Infrared Spectroelectrochemistry

Electrochemical interfaces still have remaining mysteries surrounding the interfacial region of the electrical double layer, despite being prevalent throughout the energy and water remediation industries. The electrical double layer is where many important dynamic processes such as catalysis and electron transfer occur. The goal of this work is to study the electrical double layer with two-dimensional infrared (2D IR) spectroscopy to experimentally access the details of the structural dynamics of this complex environment. However, there are several experimental challenges to applying 2D IR spectroscopy to this application, such as assuring the surface specificity of the spectrum, optimizing the signal strength while minimizing spectral distortions from dispersion and Fano line shapes, and selecting electrode materials that are both sufficiently IR compatible and conductive. Here we will discuss various considerations when designing 2D IR experiments of electrode interfaces utilizing several substrates and experimental configurations and demonstrate a robust method for 2D IR experiments of electrode interfaces under applied potential that combines nonconducting Si ATR wafers with conductive ITO and thin nanostructured films of plasmonically active Au functionalized with 3-mercapto-2-butanone (MCB). We show that layered electrodes on thin Si ATR wafers with MCB are sensitive to applied potential and that the distortions in the linear and 2D IR spectra are heavily dependent on the morphology of the Au surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗