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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 1,009 records · Page 56
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Generalized Ellipsometry Measurements of Crystalline Thin Film and Bulk Tin Oxide

Here, several bulk and thin-film crystals of SnO2 are grown and examined using generalized ellipsometry techniques. The bulk samples are grown using the chemical vapor transport technique and thin films of SnO2 are grown using the pulsed laser deposition technique. The bulk samples are examined using the two-modulator generalized ellipsometry microscope (2-MGEM) at normal incidence and the spectroscopic two-modulator generalized ellipsometer (2-MGE). The spectroscopic optical functions of tin oxide are then obtained using the 2-MGE from 1.46 to 6.2 eV. The material is highly birefringent, and the ordinary bandgap is less than the extraordinary band edge. 2-MGE measurements are also made on thin-film samples of crystalline tin oxide grown on sapphire and rutile, showing no cross polarization. Because of the complicated morphology of the tin oxide films grown on sapphire, the ellipsometry data are simulated using the Tauc–Lorentz model. Films grown on rutile had the optic axis perpendicular to the sample surface, but the film is strained, resulting in a more complicated ellipsometric spectrum. These films are modeled using the air/surface roughness/tin oxide/interface/rutile model, where the roughness and interface are modeled using the incomplete Beta function.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Nanocomposite Materials for Radionuclide Sequestration from Groundwater Environments

The half-lives of radionuclides range from fractions of a second to billions of years. Since no practical method of altering radioactive decay exists, and since exposure to either the energy emitted from radioactive decay or chemical properties of radionuclides poses dire health risks, radioactive materials must be segregated and controlled. The capture, treatment, and disposition of radioactive materials remain an extraordinary challenge. In here, we focus our attention on the synthesis and characterization of a unique class of nanocomposite materials that have potential for removal of radionuclide contamination. Specifically, we report a simple approach to decorate the surface of iron-based (Fe/FexOy) material with various nano-catalysts. Specifically, copper (Cu), tin (Sn), and silver (Ag) nanoparticles were prepared through two different reduction approaches, namely, citrate and cetyltrimethylammonium bromide (CTAB) methods, on the iron-based material surface. All samples were characterized by a variety of analytical tools, which included scanning electron microscopy (SEM), electron-dispersive X-ray microanalysis (EDS), and EDS mapping to elucidate materials’ morphology as well as nano-catalysts’ loading and location on the iron-based structures.

Hunyadi Murph, Simona E.↗
DOE OSTI2023

Modeling and mitigating fouling of microfiltration membranes for microalgae dewatering

Dewatering is energy-intensive for microalgae production, and microfiltration (MF) membranes are attractive because of their high energy efficiency. However, the membranes suffer from fouling by organic matter in the algae solutions, and there needs fundamental understanding of membrane fouling with actual algae solutions. Herein we thoroughly evaluate the dewatering performance of commercial polyethersulfone (PES) MF membranes using an integrated experiment and modeling approach. The effect of algae concentration, testing time, feed flow rate, and chemical cleaning on the dewatering performance and fouling-layer morphology are investigated. The fouling behavior can be successfully described using the Hermia and gel layer models with a gel concentration of 48 g/L for algae solutions. Furthermore, the PES membrane surface was grafted with hydrophilic zwitterions, which mitigated the fouling. For example, when challenged with 10 g/L algae solution in dead-end cells, the pristine and modified membrane exhibit water permeance of 80 and 170 L m – 2 h –1 bar –1 , respectively. Finally, three cycles of dewatering and NaOH cleaning were performed to demonstrate the promise of the MF membranes for practical dewatering application.

42 ENGINEERING↗
DOE OSTI2024

Modulating the Contact Angle between Nonpolar Polymers and SiO 2 Nanoparticles

Polymer–nanoparticle interactions play an important role in determining the morphology and properties of polymer nanocomposites and controlling the polymeric reactions involving heterogeneous catalysts. Here, in this study, we modulate the interactions between nonpolar polymers and nanoparticles by modifying the nanoparticle surface chemistry and quantify the interaction strength through direct contact angle measurements. We investigate the interactions of three nonpolar polymers, polystyrene, polyethylene, and polycyclooctene, with silica nanoparticles whose surface chemistry has been modified by atomic layer deposition of titania and calcium carbonate and by alkyl silanization. Significant differences in polymer–nanoparticle interactions are observed, which can be attributed to differences in the polarizability of the polymers and oxide surface composition. Compared to fully hydrogenated polycyclooctene, polycyclooctene is shown to have stronger interactions with most metal oxides; however, this trend is reversed following alkyl silanization of the silica nanoparticles, which makes the surface of the particles less polar. These differences in interactions can be leveraged to make polymer nanocomposites with unique properties and enable the selective conversion of polymers without the need for separations.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia

Electrochemical conversion of nitrogen to green ammonia is an attractive alternative to the Haber–Bosch process. However, it is currently bottlenecked by the lack of highly efficient electrocatalysts to drive the sluggish nitrogen reduction reaction (N2RR). In this work, we strategically design a cost-effective bimetallic Ru–Cu mixture catalyst in a nanosponge (NS) architecture via a rapid and facile method. The porous NS mixture catalysts exhibit a large electrochemical active surface area and enhanced specific activity arising from the charge redistribution for improved activation and adsorption of the activated nitrogen species. Benefiting from the synergistic effect of the Cu constituent on morphology decoration and thermodynamic suppression of the competing hydrogen evolution reaction, the optimized Ru 0.15 Cu 0.85 NS catalyst presents an impressive N 2 RR performance with an ammonia yield rate of 26.25 μg h –1 mg cat. –1 (corresponding to 10.5 μg h –1 cm –2 ) and Faradic efficiency of 4.39% as well as superior stability in alkaline medium, which was superior to that of monometallic Ru and Cu nanostructures. Additionally, this work develops a new bimetallic combination of Ru and Cu, which promotes the strategy to design efficient electrocatalysts for electrochemical ammonia production under ambient conditions.

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

Uncovering phase transformation, morphological evolution, and nanoscale color heterogeneity in tungsten oxide electrochromic materials

Controlling the electrochemical interfacial processes that govern the durability of electrochromic devices represents a key challenge in developing sustainable and cost-effective smart windows. Here, we revisit the classical tungsten trioxide (WO 3 ) materials as a platform to uncover the previously unknown interrelationship between phase transformation, morphological evolution, and nanoscale color heterogeneity in these materials. Through synchrotron/electron spectroscopic and imaging analyses, we report that the WO 3 –electrolyte interface is influenced by the tungsten dissolution and redeposition during the electrochemical cycling. The tungsten redeposition provokes the in situ crystal growth, which ultimately leads to the phase transformation from the semicrystalline WO 3 to a nanoflake-shaped, proton-trapped tungsten trioxide dihydrate (H x WO 3 · 2 H 2 O). The multidimensional quantification of the electronic structure reveals that the tungsten reduction caused by the proton trapping is heterogeneous at the nanometric scale and is responsible for the nanoscale color heterogeneity. The interplay between phase transformation, morphological evolution, and nanoscale color heterogeneity results in degraded optical modulation, switching kinetics, coulombic efficiency, and bleached-state transparency. Our results highlight that the high interfacial reactivity near the electrode surface may be the underlying mechanism for undesired bulk structural changes of electrochromic materials, and calls for fundamental studies in probing and controlling the electrode–electrolyte interfacial processes in electrochromic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Rheological dynamics and structural characteristics of supramolecular assemblies of β-cyclodextrin and sulfonic surfactants

Cyclodextrins are highly functional compounds with a hydrophobic cavity capable of forming supramolecular inclusion complexes with various classes of molecules including surfactants. The resultant rich nanostructures and their dynamics are an interesting research problem in the area of soft condensed matter and related applications. In this paper, we report novel dynamical supramolecular assemblies based on the complexation of β-cyclodextrin with 3 different sulfonic surfactants, which are sodium hexadecylsulfate, sodium dodecylbenzenesulfonate, and myristyl sulfobetaine. It was observed that a β-cyclodextrin : surfactant/2 : 1 molar ratio was ideal for inducing axial growth and imparting large viscosities in the suspensions. Such complexation processes were accompanied by intriguing nanostructural phase behaviors and rheological properties that were very sensitive to the molecular architecture of sulfonic surfactants. The presence of an amino group in the head group of the surfactant allowed for large viscosities that reached 2.4 × 10 4 Pa s which exhibited gel-like behavior. In contrast, smaller viscosity values with a lower consistency index were observed when a bulky aromatic ring was present instead. DIC microscopy was used to visually probe the microstructure of the systems with respect to sulfonate molecular architecture. Additionally, surface tension measurements, and FTIR and NMR spectroscopies were used to gain insights into the nature of interactions that lead to the complexation and nanostructural characteristics. Finally, mechanics correlating the supramolecular morphologies to the rheological properties were proposed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Response of marine post-frontal clouds to Gulf Stream variability

Understanding how Gulf Stream variation influences cloud morphology is critical for evaluating cloud feedback in the western North Atlantic Ocean and beyond, where mesoscale air-sea interactions dominate. This study investigates the impact of altered mean sea surface temperature (SST) and SST gradients on post-frontal cloud characteristics during cold-air outbreaks, using the Weather Research and Forecasting (WRF) model. Three sensitivity experiments are conducted: a control simulation (default SST), Plus4 (uniform SST increase of 4 K), and Gradplus (SST gradient enhanced by 25 %, centered around mean SST). Results reveal distinctly different responses in boundary layer dynamics and cloud macro-physics. In Plus4, a warmer and moister boundary layer reduces total cloud cover but promotes larger cloud sizes and elongated cloud streets, with diminished liquid water and enhanced ice-phase hydrometeors. Conversely, Gradplus amplifies impacts in the upwind colder SST regions, yielding a drier, colder boundary layer, weaker energy transport, and higher liquid water path but reduced ice water content and cloud lines. Tracer analysis highlights that SST modifications alter airmass sources near cloud tops due to the entrainment of ambient air, with Plus4 amplifying boundary layer contributions to cloud-top regions. These findings underscore the spatially varying effects of SST gradients and mean SST on cloud organization and microphysics, emphasizing the need to resolve ocean-atmosphere coupling in global models to improve the prediction of marine cloud feedback under warming scenarios.

AIR-SEA INTERACTION↗
DOE OSTI2021

Compressed Expanded Natural Graphite (CENG) Processing for PCM Composites

The use of phase change materials (PCMs) in thermal energy storage applications has received considerable attention in recent decades. Organic PCMs are popular due to their high latent heat of fusion, noncorrosive properties, and relative stability over many charge and discharge cycles. A primary limitation of these materials is their low thermal conductivity. This has led researchers to develop various methods to increase thermal conductivity by seeding PCM with or impregnating them into more conductive materials. One method is to impregnate PCMs into compressed expanded natural graphite (CENG) matrices, which can improve thermal conductivity by a factor of 100. CENG matrices have received particular interest due to their low cost, high porosity, small (nano/micro) pore size, high pore density, high thermal conductivity, and ability to be compressed into many geometries. PCM/CENG matrix composites have been extensively studied; however, the effect that CENG processing has on PCM saturation and the overall matrix thermal conductivity has not been well investigated. This processing includes four major steps including graphite intercalation, thermal shock, compression, and PCM saturation. Intercalation involves soaking graphite flakes in sulfuric and/or nitric acid to intercalate the acids between the graphene layers. The graphite flakes are then subjected to a high-temperature thermal shock, during which the intercalated acid is gasified rapidly, pushing the graphene layers apart, resulting in accordion-shaped graphite "worms". The "worms" are then compacted to a desired bulk density and then soaked with molten PCM until fully saturated. The properties of the produced CENG matrix, and its ability to allow PCM permeation, are sensitive to the processing parameters, namely, the thermal shock temperature and exposure time, as well as the matrix apparent density or porosity. Here, we study the effect of the thermal shock conditions necessary to expand intercalated graphite flakes on PCM saturation and the expanded graphite's thermal conductivity and morphology. We found that the thermal shock temperature exhibits the greatest influence. At greater shock temperatures, SEM images showed that expanded graphite worms exhibited greater density of pores, thus increasing total surface area within the matrices. Increasing thermal shock temperature yielded greater overall PCM saturation, as well as an increased rate of saturation. Improvements in PCM saturation rate and overall saturation are obtained as the shock temperature is increased. Longer exposure to thermal shock also improves initial saturation rates and is beneficial if a shortened impregnation time is needed. Thermal shock conditions did not impact thermal conductivity; however, conductivity was largely affected by matrix porosity. A local maximum in axial thermal conductivity was observed at around 83% porosity, which is similar to that observed in previous studies.

compressed expanded natural graphite↗
DOE OSTI2023

A UNIONS view of the brightest central galaxies of candidate fossil groups

The formation process of fossil groups (FGs) is still under debate, and, because of their relative rarity, large samples of such objects are still missing. The aim of the present paper is to increase the sample of known FGs, to analyse the properties of their brightest group galaxies (BGGs), and to compare them with a control sample of non-FG BGGs. We extracted a sample of 87 FG and 100 non-FG candidates from a large spectroscopic catalogue of haloes and galaxies. For all the objects with data available in UNIONS (initially the Canada France Imaging Survey, CFIS) in the u and r bands, and/or in an extra r-band processed to preserve all low-surface-brightness features (rLSB), we performed a 2D photometric fit of the BGG with GALFIT with one or two Sérsic components. We also analysed how the subtraction of the intracluster light (ICL) contribution modifies the BGG properties. From the SDSS spectra available for the BGGs of 65 FGs and 82 non-FGs, we extracted the properties of their stellar populations with Firefly. To complement our study, and in order to provide a detailed illustration of the possible origin of emission lines in the FG BGGs, involving the presence or absence of an AGN, we investigated the origin of the emission lines in a nearby FG that is dominated by the NGC 4104 galaxy. Morphologically, a single Sérsic profile can fit most objects in the u band, while two Sérsics are needed in the r and rLSB bands, both for FGs and non-FGs. Non-FG BGGs cover a larger range of Sérsic index n. FG BGGs follow the Kormendy relation (mean surface brightness versus effective radius) previously derived for almost 1000 brightest cluster galaxies (BCGs), while the majority of non-FGs BGGs are located below this relation, with fainter mean surface brightnesses. This suggests that FG BGGs have evolved similarly to BCGs, and non-FG BGGs have evolved differently from both FG BGGs and BCGs. All the above properties can be strongly modified by the subtraction of the ICL contribution. Based on spectral fitting, the stellar populations of FG and non-FG BGGs do not differ significantly. FG and non-FG BGGs differ from one another in terms of their morphological properties and Kormendy relation, suggesting they have had different formation histories. However, it is not possible to trace differences in their stellar populations or in their large-scale distributions.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Hunting for Planetary Nebulae toward the Galactic Center

We present near-infrared (IR) spectra of two planetary nebula (PN) candidates in close lines of sight toward the Galactic center (GC) using the Gemini Near-Infrared Spectrograph at Gemini North. High-resolution images from radio continuum and narrowband IR observations reveal ringlike or barrel-shaped morphologies of these objects, and their mid-IR spectra from the Spitzer Space Telescope exhibit rich emission lines from highly-excited species such as [S iv], [Ne iii], [Ne v], and [O iv]. We also derive elemental abundances using the Cloudy synthetic models, and find an excess amount of the s-process element krypton in both targets, which supports their nature as PNe. We estimate foreground extinction toward each object using near-IR hydrogen recombination lines, and find significant visual extinctions (A {sub V} > 20). The distances inferred from the size versus surface brightness relation of other PNe are 9.0 ± 1.6 kpc and 7.6 ± 1.6 kpc for SSTGC 580183 and SSTGC 588220, respectively. These observed properties along with the abundance patterns and close proximity to Sgr A* (projected distances ≲20 pc) make it highly probable that these objects are the first confirmed PN objects in the nuclear stellar disk. The apparent scarcity of such objects resembles the extremely low rate of PN formation in old stellar systems, but is in line with the current rate of sustained star formation activity in the Central Molecular Zone.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Impact of mixed grain size sediment input on braided river Morphodynamics: Insights from experimental and numerical modeling

The rate of sediment supply has significant impacts on river morphology, making it crucial to understand the geomorphic changes and grain size distribution dynamics in rivers. However, the effects of varying grain size sediment input on morphological changes in braided channels remain poorly understood. This study is the first to investigate the bar development and sediment sorting processes in braided channels with non-uniform sediment inputs using both numerical and experimental approaches. We applied a two-dimensional numerical model, Nays2DH to confirm and generalize experimental results. The model reproduced key experiment results, including 1) stream elevation changes, and 2) grain size distribution. Using this validated model, we explored the morphological changes and sorting process in a braided river with sediment inputs. The numerical experiments demonstrate that sediment input controls the elevation of the stream bed and the grain size distribution. Notably, both the elevation and grain-size distribution become relatively stable in downstream of the channel. Additionally, the simulation results suggest that an increased sediment supply leads to greater channel complexity, with bed surface armoring decreasing.

Nays2DH↗
DOE OSTI2021

Incorporation of Ti in epitaxial Fe2TiO4 thin films

The titanomagnetites (Fe2-xTixO4, x = 1) are a family of reducible spinel-structure oxides of interest for their favorable magnetic, catalytic, and electrical transport properties. To understand the stability of the system during low temperature deposition, epitaxial thin films of Fe2TiO4 were deposited by molecular beam epitaxy on MgO(001) at 250 – 375°C. The homogeneous incorporation of Ti, Fe valence, and film morphology were all found to be strongly dependent on the oxidation conditions at the low substrate temperatures employed. More oxidizing conditions led to phase separation into epitaxial, faceted Fe3O4 and rutile TiO2. Less oxidizing conditions resulted in polycrystalline films that exhibited Ti segregation to the film surface, as well as mixed Fe valence (Fe3+, Fe2+, Fe0). A narrow window of intermediate oxygen partial pressure during deposition yielded nearly homogeneous Ti incorporation and a large fraction of Fe2+. However, these films were poorly crystallized, and no occupation of tetrahedral sites in the spinel lattice by Fe2+ was detected by x-ray magnetic circular dichroism at the Fe L-edge. After vacuum annealing, a small fraction of Fe2+ was found to occupy tetrahedral sites. Comparison of these results with previous work suggests that the restriction of the deposition conditions to low temperature by the MgO substrate limits the incorporation of Ti into the spinel lattice. This work suggests a path towards obtaining stoichiometric, well-crystallized Fe2TiO4 by MBE by utilizing high substrate temperature and low oxygen partial pressure during deposition on temperature-stable substrates.

Kaspar, Tiffany C.↗
DOE OSTI2025

Designing Physicochemically‐Ordered Interphases for High‐Performance Composites

To enhance the mechanical properties of carbon fiber‐reinforced polymer composites, a physicochemical scaffold is designed incorporating microscopically architected chemically reactive nanofibers that act as a multiscale bridge between the carbon fibers and the matrix. Thermally activated nanofibers leverage their morphologically driven mechanochemical properties to form covalent bonds with adjacent polymer molecules, creating a co‐continuous network that dramatically enhances fiber‐matrix load transfer. By meticulously controlling the nanofiber architecture through variable surface area, functional group availability, and polymer chain alignment effects, the extent of covalent bonding between nanofibers and the matrix is manipulated ultimately resulting in improved carbon fiber‐matrix adhesion. Further, the concept was validated using polyacrylonitrile nanofibers within an acrylonitrile butadiene styrene matrix in a discontinuous carbon fiber‐reinforced composite system. Nanomechanical studies using atomic force microscopy and low‐field nuclear magnetic resonance spectroscopy confirmed immobilized, chemically transferred, and ordered nanostructures at the interphase. The resulting composites demonstrated ≈56% and ≈175% improvements in tensile strength and toughness, respectively, compared to composites without nanofiber. Comprehensive thermal, rheological, and X‐ray scattering analyses, along side all‐atomic molecular dynamics simulations, revealed the fundamental mechanisms behind these improvements in mechanical behavior. The versatility and efficacy of the approach have the potential to address longstanding interphase challenges in the composite industry.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Conservative solute transport processes and associated transient storage mechanisms: Comparing streams with contrasting channel morphologies, land use and land cover

Abstract Land use within a watershed impacts stream channel morphology and hydrology and, therefore, in‐stream solute transport processes and associated transient storage mechanisms. This study evaluated transport processes in two contrasting stream sites where channel morphology was influenced by the surrounding land use, land cover, climate and geologic controls: Como Creek, CO, a relatively undisturbed, high gradient, forested stream with a gravel bed and complex channel morphology, and Clear Creek, IA, an incised, low‐gradient stream with low‐permeability substrate draining an agricultural landscape. We performed conservative stream tracer injections at these sites to address the following questions: (1) How does solute transport vary between streams with differing morphologies? and (2) How does solute transport at each stream site change as a function of discharge? We analysed in‐stream tracer time series data and compared results quantifying solute attenuation in surface and subsurface transient storage zones. Significant trends were observed in these metrics with varying discharge conditions at the forested site but not at the agricultural site. There was a broad range of transport mechanisms and evidence of substantial exchange with both surface and hyporheic transient storage in the relatively undisturbed, forested stream. Changing discharge conditions activated or deactivated different solute transport mechanisms in the forested site and greatly impacted advective travel time. Conversely in the simplified agricultural stream, there was a narrow range of solute transport behaviour across flows and predominantly surface transient storage at all measured discharge conditions. These results demonstrate how channel simplification inhibits available solute transport mechanisms across varying discharge conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

A novel approach to identify the ionomer phase in PEMFC by EELS

Proton exchange membrane fuel cells are one of the most promising technologies of energy conversion for both automotive and stationary applications, due to their ultimate cleanness and high efficiency. A critical factor, which strongly affects the fuel cell performance, is the ionomer distribution and coverage over the carbon support, since the catalysts, which are typically Pt and/or Pt-alloy nanoparticles, must be located at the carbon support/ionomer interface to catalyze the sluggish oxygen reduction reaction. However, the characterization and identification of the ionomer film, in terms of ionomer distribution and coverage over the carbon surface, is a long standing challenge. This is because the ionomer film may suffer from beam damage during the characterization, either from x-rays, neutrons or an electron beam, which causes morphological changes. In this regard, we report here a novel approach to identify and differentiate the ionomer, using the carbon signal produced by STEMEELS. Using this approach, not only the ionomer distribution, but also the carbon support distribution, can be probed at high spatial resolutions. In addition, this new approach allows us to identify ionomer-rich and carbon-support rich regions, which are quite challenging to determine using other methods.

08 HYDROGEN↗
DOE OSTI2025

Directed Synthesis of Gold Nanoparticle Superstructures Using Self-Assembling Peptoids Containing Metal-Bonding N-Heterocyclic Carbenes

N-Heterocyclic carbene (NHC) ligands, with strong metal-binding affinity, offer a robust platform for constructing organic–inorganic nanohybrids with high stability and tunable properties. However, achieving precise structural control in a simple manner remains challenging. Here, we report a one-pot synthesis of nanohybrids using self-assembling peptoids functionalized with histidine-2-ylidene, which simultaneously enable peptoid assembly and NHC–metal binding. Histidine-2-ylidene-functionalized peptoids were designed to self-assemble and provide NHC binding sites, while AuNPs served as the inorganic component due to NHCs’ strong affinity for gold surfaces. The resulting peptoid-NHC@AuNPs form well-defined vesicles that are characterized by UV–vis spectroscopy, X-ray photoelectron spectroscopy, and electron microscopy. Importantly, the vesicle size and morphology can be tuned via the peptoid sequence or environmental conditions. Further experiments highlight the crucial role of the NHC sites in the formation and stabilization of these nanohybrids. This modular strategy offers a versatile route to fabricating functional NHC-based nanohybrids for potential applications in sensing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Physicochemical Heterogeneity in Silicon Anodes from Cycled Lithium-Ion Cells

The severe capacity fade of lithium-ion cells with silicon-dominant anodes has hindered their widescale commercialization. In this work, we link cell capacity fade to the heterogeneous physicochemical evolution of silicon anodes during battery cycling. Through a multi-length scale characterization approach, we demonstrate that silicon particles near the anode surface react differently than those near the copper current collector. In particular, near the anode surface we find an amorphized wispy silicon encased in a highly fluorinated matrix of electrolyte-reduction products. In contrast, closer to the current collector, the silicon retains more of its initial morphology and structure, suggesting the presence of isolated particles. Here, the results show that accessibility of active silicon to lithium-ions varies across the anode matrix. Material and cell designs, which minimize electrode expansion resulting from the in-filling of pores with the solid electrolyte interphase (SEI), are needed to enhance anode homogeneity during the electrochemical cycling.

25 ENERGY STORAGE↗