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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 991 records · Page 55
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Solid-state polymer-particle hybrid electrolytes: Structure and electrochemical properties

Solid-state electrolytes (SSEs) are challenged by complex interfacial chemistry and poor ion transport through the interfaces they form with battery electrodes. Here, we investigate a class of SSE composed of micrometer-sized lithium oxide (Li 2 O) particles dispersed in a polymerizable 1,3-dioxolane (DOL) liquid. Ring-opening polymerization (ROP) of the DOL by Lewis acid salts inside a battery cell produces polymer-inorganic hybrid electrolytes with gradient properties on both the particle and battery cell length scales. These electrolytes sustain stable charge-discharge behavior in Li||NCM811 and anode-free Cu||NCM811 electrochemical cells. On the particle length scale, Li 2 O retards ROP, facilitating efficient ion transport in a fluid-like region near the particle surface. On battery cell length scales, gravity-assisted settling creates physical and electrochemical gradients in the hybrid electrolytes. By means of electrochemical and spectroscopic analyses, we find that Li 2 O particles participate in a reversible redox reaction that increases the effective CE in anode-free cells to values approaching 100%, enhancing battery cycle life.

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

Dual 3D Ceramic Textile Electrodes: Fast Kinetics for Carbon Oxidation Reaction and Oxygen Reduction Reaction in Direct Carbon Fuel Cells at Reduced Temperatures

Abstract Direct carbon fuel cells (DCFCs) are an efficient energy‐conversion technology capable of generating electricity with carbon‐dioxide‐capture chemistry with solid carbon as fuels. The efficiency and performance of DCFCs depend on the kinetics of the carbon oxidation reactions (COR) and the oxygen reduction reactions (ORR), each occurring at anode and cathode, respectively. The limited active sites paired with reduced temperatures greatly decrease the efficiency of the electrochemical reactions. Ultraporous dual‐3D ceramic textiles (dual‐3DCT) are integrated into electrolyte‐supported DCFCs to enhance charge and mass transfer at the electrodes. Improved COR at the anode is achieved by the synergy between the 3DCT NiO–Ce 0.8 Gd 0.2 O 1.95 (GDC) structure and optimal carbon fuel choice. In a comparative study, DCFCs using graphitic carbon (GC) as fuel show the best COR performance when compared to DCFCs utilizing alternative fuels such as carbon black (CB) and activated carbon (AC). The 3DCT Sm 0.5 Sr 0.5 CoO 3‐δ –GDC (SSC–GDC) composite cathode shows electrochemical performance superior to that of the conventional screen‐printed SSC–GDC. A peak power density of 392 mW cm −2 at 600 °C is obtained in a DCFC using the 3DCT‐anode/electrolyte/3DCT‐cathode configuration, an unprecedented value for any reported DCFC as of yet. This points toward promising applications of dual‐3DCT electrodes for reduced‐temperature DCFCs.

Bian, Wenjuan↗
DOE OSTI2020

Maximizing ion accessibility in MXene-knotted carbon nanotube composite electrodes for high-rate electrochemical energy storage

Improving the accessibility of ions in the electrodes of electrochemical energy storage devices is vital for charge storage and rate performance. In particular, the kinetics of ion transport in organic electrolytes is slow, especially at low operating temperatures. Herein, we report a new type of MXene-carbon nanotube (CNT) composite electrode that maximizes ion accessibility resulting in exceptional rate performance at low temperatures. The improved ion transport at low temperatures is made possible by breaking the conventional horizontal alignment of the two-dimensional layers of the MXene Ti 3 C 2 by using specially designed knotted CNTs. The large, knot-like structures in the knotted CNTs prevent the usual restacking of the Ti 3 C 2 flakes and create fast ion transport pathways. The MXene-knotted CNT composite electrodes achieve high capacitance (up to 130 F g -1 (276 F cm -3 )) in organic electrolytes with high capacitance retention over a wide scan rate range of 10 mV s -1 to 10 V s -1 . This study is also the first report utilizing MXene-based supercapacitors at low temperatures (down to -60 °C).

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

N-Doped Graphene (N-G)/MOF(ZIF-8)-Based/Derived Materials for Electrochemical Energy Applications: Synthesis, Characteristics, and Functionality

In recent years, graphene-type materials originating from metal–organic frameworks (MOFs) or integrated with MOFs have exhibited notable performances across various applications. However, a comprehensive understanding of these complex materials and their functionalities remains obscure. While some studies have reviewed graphene/MOF composites from different perspectives, due to their structural–functional intricacies, it is crucial to conduct more in-depth reviews focusing on specific sets of graphene/MOF composites designed for particular applications. In this review, we thoroughly investigate the syntheses, characteristics, and performances of N-G/MOF(ZIF-8)-based/derived materials employed in electrochemical energy conversion and storage systems. Special attention is given to realizing their fundamental functionalities. The discussions are divided into three segments based on the application of N-G/ZIF-8-based/derived materials as electrode materials for batteries, electrodes for electrochemical capacitors, and electrocatalysts. As electrodes for batteries, N-G/MOF(ZIF-8) materials can mitigate issues like an electrode volume expansion for Li-ion batteries and the ‘shuttle effect’ for Li-S batteries. As electrodes for electrochemical capacitors, these materials can considerably improve the ion transfer rate and electronic conductivity, thereby enhancing the specific capacitance while maintaining the structural stability. Also, it was observed that these materials could occasionally outperform standard platinum-based catalysts for the electrochemical oxygen reduction reaction (ORR). The reported electrochemical performances and structural parameters of these materials were carefully tabulated in uniform units and scales. Through a critical analysis of the present synthesis trends, characteristics, and functionalities of these materials, specific aspects were identified that required further exploration to fully utilize their inherent capabilities.

Electrochemistry↗
NASA NTRS1985

Structure-property characterization of rheocast and VADER processed IN-100 superalloy

Two recent solidification processes have been applied in the production of IN-100 nickel-base superalloy: rheocasting and vacuum arc double electrode remelting (VADER). A detailed microstructural examination has been made of the products of these two processes; associated tensile strength and fatigue crack propagation (FCP) rate at an elevated temperature were evaluated. In rheocasting, processing variables that have been evaluated include stirring speed, isothermal stirring time and volume fraction solid during isothermal stirring. VADER processed IN-100 was purchased from Special Metals Corp., New Hartford, NY. As-cast ingots were subjected to hot isostatic pressing (HIP) and heat treatment. Both rheocasting and VADER processed materials yield fine and equiaxed spherical structures, with reduced macrosegregation in comparison to ingot materials. The rheocast structures are discussed on the basis of the Vogel-Doherty-Cantor model of dendrite arm fragmentation. The rheocast ingots evaluated were superior in yield strength to both VADER and commercially cast IN-100 alloy. Rheocast and VADER ingots may have higher crack propagation resistance than P/M processed material.

Cheng, J. J. A.↗
DOE OSTI2024

Structural modeling of high-entropy oxides battery anodes using x-ray absorption spectroscopy

High-entropy oxides (HEOs) are single phase solid solutions where five or more metals share the same sublattice, giving rise to unexpected features in various fields of applications. Recently, HEOs have emerged as an alternative conversion electrode anode material for next-generation Li-ion batteries, where the combination of several different elements in a single solid solution can synergistically act to overcome some of its main drawbacks, improving performance. Due to their chemical complexity, x-ray absorption spectroscopy (XAS) emerges as an appropriate technique to study the electronic (x-ray absorption near edge structure, XANES) and local structure (extended x-ray absorption fine structure, EXAFS) of these compounds as a function of cycling. This work aims to highlight the capabilities of XAS as an element-specific probe to understand a material’s structure at the atomistic level through EXAFS modeling of (MgFeCoNiCuZn)O high-entropy system and how to extract valuable information about the bond distance, number of near neighbors, and local disorder, which are crucial to a full understanding of the electrochemical reaction mechanisms of such battery electrodes.

25 ENERGY STORAGE↗
DOE OSTI2022

Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands

Tailoring electron transfer dynamics across solid–liquid interfaces is fundamental to the interconversion of electrical and chemical energy. Stacking atomically thin layers with a small azimuthal misorientation to produce moiré superlattices enables the controlled engineering of electronic band structures and the formation of extremely flat electronic bands. Here, we report a strong twist-angle dependence of heterogeneous charge transfer kinetics at twisted bilayer graphene electrodes with the greatest enhancement observed near the ‘magic angle’ (~1.1°). Furthermore, this effect is driven by the angle-dependent tuning of moiré-derived flat bands that modulate electron transfer processes with the solution-phase redox couple. Combined experimental and computational analysis reveals that the variation in electrochemical activity with moiré angle is controlled by a structural relaxation of the moiré superlattice at twist angles of <2°, and ‘topological defect’ AA stacking regions, where flat bands are localized, produce a large anomalous local electrochemical enhancement that cannot be accounted for by the elevated local density of states alone.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Integrated Reference Electrodes in Anion-Exchange-Membrane Electrolyzers: Impact of Stainless-Steel Gas-Diffusion Layers and Internal Mechanical Pressure

Alkaline-membrane electrolyzers operating in pure water might provide scalable low-cost H 2 production but currently lag in performance and durability compared to commercial technologies. Typically, membrane–electrode assemblies (MEAs) are optimized in electrolyzers by changing one parameter at a time and assessing the resulting system performance via two-electrode polarization and impedance measurements. These approaches are limited in their ability to assign performance changes and durability to specific electrodes or processes. We integrate a reference electrode with the MEA to separate anode and cathode responses in both polarization and impedance measurements. Here we illustrate the power of the approach by showing how the fiber diameter of stainless-steel gas-diffusion layers (GDLs) affects performance solely at the anode, while changing the thickness of the cathode GDL simultaneously affects the performance of the anode and cathode due to changes in internal pressure from mechanical compression. This finding was obscured in conventional two-electrode measurements. The work thus guides both high-performance alkaline-membrane water-electrolyzer development and illustrates a useful strategy to study structure–activity relationships in the MEA.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Effects of Ink Formulation on Construction of Catalyst Layers for High-Performance Polymer Electrolyte Membrane Fuel Cells

Rational design of catalyst layers in a membrane electrode assembly (MEA) is crucial for achieving high-performance polymer electrolyte membrane fuel cells. Establishing a clear understanding of the property (catalyst ink)–structure (catalyst layer)–performance (MEA) relationship lays the foundation for this rational design. Here, a synergistic approach was taken to correlate the ink formulation, the microstructure of catalyst layers, and the resulting MEA performance to establish such a property–structure–performance relationship. The solvent composition (n-PA/H 2 O mixtures) demonstrated a strong influence on the performance of the MEA fabricated with an 830-EW (Aquivion) ionomer, especially polarization losses of cell activation and mass transport. The performance differences were studied in terms of how the solvent composition affects the catalyst/ionomer interface, ionomer network, and pore structure of the resulting catalyst layers. The ionomer aggregates mainly covered the surface of catalyst aggregates acting as oxygen reduction reaction active sites, and the aggregate sizes of the ionomer and catalyst (revealed by ultrasmall angle X-ray scattering and cryo-transmission electron microscopy) were dictated by tuning the solvent composition, which in turn determined the catalyst/ionomer interface (available active sites). In n-PA/H 2 O mixtures with 50~90 wt % H 2 O, the catalyst agglomerates could be effectively broken up into small aggregates, leading to enhanced kinetic activities. The boiling point of the mixed solvents determined the pore structure of ultimate catalyst layers, as evidenced by mercury porosimetry and scanning electron microscopy. For mixed solvents with a higher boiling point, the catalyst–ionomer aggregates in the ink tend to agglomerate during the solvent evaporation process and finally form larger catalyst–ionomer aggregates in the ultimate catalyst layer, resulting in more secondary pores and thus lower mass transport resistance. Both the enlarged catalyst/ionomer interface and appropriate pore structure were achieved with the catalyst layer fabricated from an n-PA/H 2 O mixture with 90 wt % H 2 O, leading to the best MEA performance.

25 ENERGY STORAGE↗
DOE OSTI2020

Nano-Ceramic Cathodes via Co-sputtering of Gd–Ce Alloy and Lanthanum Strontium Cobaltite for Low-Temperature Thin-Film Solid Oxide Fuel Cells

We report the electrochemical performance and structural characteristics of porous nanostructured ceramic cathodes for thin-film solid oxide fuel cells (TF-SOFCs) based on yttria-stabilized zirconia (YSZ) electrolytes. The nanostructured cathode is obtained through magnetron co-sputtering of gadolinium–cerium (Gd–Ce) alloy and lanthanum strontium cobaltite perovskite targets. The resultant nanostructure and composition of the ceramic cathode are controlled by adjusting the co-sputtering conditions. The peak power densities in our fabricated TF-SOFCs are the highest reported values for YSZ-based electrolyte SOFCs, showing 0.14, 0.48, 1.21, 2.56, and 3.01 W/cm2 at 450, 500, 550, 600, and 650 °C, respectively, operating under air and pure hydrogen fuel. The results show that the porosity and composition of the cathode greatly affect the resulting peak power densities. This work illustrates the capability of sputtering to produce stable, scalable, nano-ceramic cathodes with superb peak power densities when integrated in TF-SOFCs.

25 ENERGY STORAGE↗
DOE OSTI2024

Elucidation of Design Criteria for V‐based Redox Mediators: Structure‐Function Relationships that Dictate Rates of Heterogeneous Electron Transfer

Redox mediators are attractive solutions for addressing the stringent kinetic stipulations required for efficient energy conversion processes. In this work, we compare the electrochemical properties of four vanadium complexes, namely [V(acac) 3 ], [V 6 O 7 (OMe) 12 ], [ n Bu 4 N] 3 [V 6 O 13 (TRIS NO2 ) 2 ], and [ n Bu 4 N] 5 [V 18 O 46 (NO 3 )] in non-aqueous solutions on glassy carbon electrodes. The goal of this study is to investigate the electron transfer kinetics and diffusivity of these compounds under identical experimental conditions to develop an understanding of structure-function relationships that dictate the physicochemical properties of vanadium oxide assemblies. Complex selection was dictated by two criteria – (1) nuclearity of the transition metal complexes (2) distribution of electron density in the native electronic configuration. In conclusion, our analyses establish that electronic communication between metal centers significantly impacts charge transfer kinetics of these vanadium-based compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Investigating instabilities in magnetized low-pressure capacitively coupled RF plasma using particle-in-cell (PIC) simulations

The effect of a uniform magnetic field on particle transport in low-pressure radio frequency (RF) capacitively coupled plasma (CCP) has been studied using a particle-in-cell model. Three distinct regimes of plasma behavior can be identified as a function of the magnetic field. In the first regime at low magnetic fields, asymmetric plasma profiles are observed within the CCP chamber due to the effect of $\overrightarrow{E}$ × $\overrightarrow{B}$ drift. As the magnetic field increases, instabilities develop and form self-organized spoke-shaped structures that are distinctly seen within the bulk plasma closer to the sheath. In this second regime, the spoke-shaped coherent structures rotate inside the plasma chamber in the -$\overrightarrow{E}$ × $\overrightarrow{B}$ direction, where $\overrightarrow{E}$ × $\overrightarrow{B}$ are the DC electric and magnetic field vectors, respectively, and the DC electric field exists in the sheath and pre-sheath regions. The spoke rotation frequency is in the megahertz range. As the magnetic field strength increases further, the rotating coherent spokes continue to exist near the sheath. The coherent structures are, however, accompanied by new small-scale incoherent structures originating and moving within the bulk plasma region away from the sheath. This is the third regime of plasma behavior. The threshold values of the magnetic field between these regimes were found not to vary with changing plasma reactor geometry (e.g., area ratio between ground and powered electrodes) or the use of an external capacitor between the RF-powered electrode and the RF source. The threshold values of the magnetic field between these regimes shift toward higher values with increasing gas pressure. Analysis of the results indicates that the rotating structures are due to the lower hybrid instability driven by density gradients and electron-neutral collisions. This paper provides guidance on the upper limit of the magnetic field for instability-free operation in low-pressure CCP-based semiconductor deposition and etch systems that use the external magnetic field for plasma uniformity control.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Multiscale operando X-ray investigations provide insights into electro-chemo-mechanical behavior of lithium intercalation cathodes

The electrochemical performance and cycle life of lithium-ion batteries (LIBs) depend on the electrochemical, chemical, and mechanical behavior of electrodes and electrolytes. Despite extensive studies conducted previously, challenges exist to decouple these behaviors, capture the evolution of electro-chemo-mechanical behavior in realistic conditions, and correlate atomic-scale stress evolution to micro-scale bulk mechanical degradation. Here, we report multiscale operando techniques to investigate polydisperse battery electrodes by integrating volume-averaged quantitative synchrotron X-ray scattering with high-resolution transmission X-ray microscopy (TXM). The former provides us information spanning a wide spatial range, from Angstrom-level atomic structures to micrometer-level particle scales, while the latter provides time-resolved 2D images of the particles during cycling. The complementarity of the two operando techniques is demonstrated by an over-lithiation test of LiCoO 2 electrodes, where particles crack and eventually pulverize. Additionally, the techniques are applied to study LiCoO 2 cycling stability from 3.0 V to 4.5 V. Operando X-ray scattering result shows nanometer-scale features keep forming in LiCoO 2 electrodes during cycling, resulting in an increased projected area observed by the TXM experiment. The formation of such features is inhibited by a polymer coating on the electrode, leading to vastly improved cycling stability. The polymer coating alleviates LiCoO 2 surface deterioration, reduces side product generation, and inhibits LiCoO 2 particles volume expansion during the cycling test. These operando multimodal X-ray techniques presented herein thus offer a novel, multiscale diagnostic modality for studying existing and emerging battery materials, aiding the development of next-generation LIBs.

25 ENERGY STORAGE↗
DOE OSTI2020

Bismuthene for highly efficient carbon dioxide electroreduction reaction

Bismuth (Bi) has been known as a highly efficient electrocatalyst for CO 2 reduction reaction. Stable free-standing two-dimensional Bi monolayer (Bismuthene) structures have been predicted theoretically, but never realized experimentally. Here, we show the first simple large-scale synthesis of free-standing Bismuthene, to our knowledge, and demonstrate its high electrocatalytic efficiency for formate (HCOO - ) formation from CO 2 reduction reaction. The catalytic performance is evident by the high Faradaic efficiency (99% at -580 mV vs. Reversible Hydrogen Electrode (RHE)), small onset overpotential (<90 mV) and high durability (no performance decay after 75 h and annealing at 400 °C). Density functional theory calculations show the structure-sensitivity of the CO2 reduction reaction over Bismuthene and thicker nanosheets, suggesting that selective formation of HCOO - indeed can proceed easily on Bismuthene (111) facet due to the unique compressive strain. This work paves the way for the extensive experimental investigation of Bismuthene in many different fields.

Science & Technology - Other Topics↗
DOE OSTI2022

Filament Formation in TaO x Thin Films for Memristor Device Application: Modeling Electron Energy Loss Spectra and Electron Transport

Abstract Although understanding filament formation in oxide‐based memristive devices by theory has emerged, there are still fundamental unanswered questions. Importantly, for practical application of thin films the material in its amorphous state is to be considered, but mostly lacking so far, and details on sub‐stoichiometry are also scarce. To gain insight into the optical and electronic properties of sub‐stoichiometric amorphous tantalum oxide (TaO x ), the electron energy loss spectrum (EELS) of model systems is characterized theoretically and electron transport characteristics are analyzed in detail. Calculated blue‐shifts by increasing sub‐stoichiometry explained the measurements, potentially suggesting estimation of oxygen vacancy concentrations through EEL spectra. Electron transport results based on TaO x material models validated by EELS measurements show that oxygen vacancy filamentary paths are initiated at low bias upon increasing sub‐stoichiometry yet noting an interplay with the local amorphous structure. Contact resistances at interfaces of the TaO x switching layer and a tantalum scavenging layer or titanium nitride electrode are quantified, indicating the possibility for either oxygen vacancy‐ or metal cluster‐based conduction mechanisms at the interface. The computational work, combined with experimental characterization for validation, provides a basis for investigating effects of sub‐stoichiometry on filament formation in TaO x thin film memristive devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Reversible (De)Intercalation of Hydrated Zn 2+ in Mg 2+ -Stabilized V 2 O 5 Nanobelts with High Areal Capacity

The rechargeable aqueous zinc ion battery (ZIB) is regarded as one of the most promising candidates for large-scale energy storage applications due to its low-cost and eco-friendly properties. However, the development of a suitable cathode operating with high areal capacity and uncovering the relevant reaction mechanisms remain challenging. Herein, the application of Mg 0.26 V 2 O 5 ∙0.73H 2 O (MVO) nanobelts as a ZIB cathode is demonstrated. In situ FT-IR reveals the shift of OH stretching from 3350 cm -1 to 3200 cm -1 , corresponding to the hydration shell of Zn 2+ , while in situ Raman suggests the interlayer charges creening effect, which would boost the intercalation of hydrated Zn 2+ . Density function theory reveals that the hydrated Zn 2+ can lower the Coulombic repulsion at the electrode-electrolyte interface and circumvents the desolvation penalty of hydrated Zn 2+ during the (de)intercalation process. Additionally, excellent structure stability and large interlayer spacing guarantee the highly reversible (de)intercalation of hydrated Zn 2+ . Therefore, the MVO nanobelts exhibit a high areal capacity of 2.12 mAh cm -2 at 0.05 A g -1 , outstanding cycling stability of 2500 cycles at 10 A g -1 with a mass loading of 5 mg cm -2 . Finally, it is believed that the use of hydrated intercalation charge carriers will boost further studies in other multivalent rechargeable batteries.

25 ENERGY STORAGE↗
DOE OSTI2021

Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Polymer–Particle Interactions and Spinnability

We investigate the effect of the poly(acrylic acid) (PAA) carrier polymer concentration on the microstructure and rheological properties of catalyst inks for electrospun polymer–electrolyte membrane fuel-cell catalyst layers. Characterization of an ink microstructure using oscillatory shear rheology showed that the catalyst particles (platinum on carbon) are significantly agglomerated in the absence of PAA or an ionomer. Both the ionomer and PAA promoted the stability of the particles against agglomeration via electrosteric stabilization by adsorbing onto the particle surface. Increasing the PAA concentration increased the stability of the particles (or reduced the agglomerated structure) due to increasing PAA coverage onto the free surface area of the particles. However, beyond a certain increase in concentration, PAA was found to predominantly remain as an excess free polymer in the ink due to an insufficient free/available surface area on the particles for further PAA coverage. Extensional rheology measurements demonstrated that PAA enhances the extensional viscosities of the inks. Consequently, increasing the PAA concentration in the ink promoted the evolution of uniform nanofibers. However, beyond a certain concentration, a significant increase in the shear viscosities of the inks led to defective fiber morphologies because of the onset of flow instabilities. Electrochemical performance comparisons between catalyst layers with different PAA concentrations showed maximum performance at the PAA concentration that led to the least agglomerated structure of the catalyst, most uniform fiber morphologies, and low concentrations of free (non-adsorbing) PAA in the electrode. These results provide a rationale for optimization of electrospun catalyst nanofibers for both spinnability and electrochemical performance.

25 ENERGY STORAGE↗
DOE OSTI2023

The Effect of the SEI Layer Mechanical Deformation on the Passivity of a Si Anode in Organic Carbonate Electrolytes

The solid electrolyte interphase (SEI) on a Si negative electrode in carbonate-based organic electrolytes shows intrinsically poor passivating behavior, giving rise to unsatisfactory calendar life of Li-ion batteries. Moreover, mechanical strains induced in the SEI due to large volume changes of Si during charge-discharge cycling could contribute to its mechanical instability and poor passivating behavior. This study elucidates the influence that static mechanical deformation of the SEI has on the rate of unwanted parasitic reactions at the Si/electrolyte interface as a function of electrode potential. Further, the experimental approach involves the utilization of Si thin-film electrodes on substrates with disparate elastic moduli, which either permit or suppress the SEI deformation in response to Si volume changes upon charging-discharging. We find that static mechanical stretching and deformation of the SEI results in an increased parasitic electrolyte reduction current on Si. Furthermore, attenuated total reflection and near-field Fourier-transform infrared nanospectroscopy reveal that the static mechanical stretching and deformation of the SEI fosters a selective transport of linear carbonate solvent through, and nanoconfinement within, the SEI. These, in turn, promote selective solvent reduction and continuous electrolyte decomposition on Si electrodes, reducing the calendar life of Si anode-based Li-ion batteries. Finally, possible correlations between the structure and chemical composition of the SEI layer and its mechanical and chemical resilience under prolonged mechanical deformation are discussed in detail.

25 ENERGY STORAGE↗