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At least 397 records · Page 22

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DOE OSTI2024

Tracking copper nanofiller evolution in polysiloxane during processing into SiOC ceramic

Polymer-derived ceramics (PDCs) remain at the forefront of research for a variety of applications including ultra-high-temperature ceramics, energy storage and functional coatings. Despite their wide use, questions remain about the complex structural transition from polymer to ceramic and how local structure influences the final microstructure and resulting properties. This is further complicated when nanofillers are introduced to tailor structural and functional properties, as nanoparticle surfaces can interact with the matrix and influence the resulting structure. The inclusion of crystalline nanofiller produces a mixed crystalline–amorphous composite, which poses characterization challenges. With this study, we aim to address these challenges with a local-scale structural study that probes changes in a polysiloxane matrix with incorporated copper nanofiller. Composites were processed at three unique temperatures to capture mixing, pyrolysis and initial crystallization stages for the pre-ceramic polymer. We observed the evolution of the nanofiller with electron microscopy and applied synchrotron X-ray diffraction with differential pair distribution function (d-PDF) analysis to monitor changes in the matrix's local structure and interactions with the nanofiller. The application of the d-PDF to PDC materials is novel and informs future studies to understand interfacial interactions between nanofiller and matrix throughout PDC processing.

Chemistry↗

DOE OSTI2024

Morphological Evolution and Dealloying During Corrosion of Ni20Cr (wt.%) in Molten FLiNaK Salts

The dealloying corrosion behavior of the FCC Ni20Cr (wt%) in molten LiF-NaF-KF (FLiNaK) salts at 600 °C under varying applied potentials was investigated. Using in-operando electrochemical techniques and a multi-modal suite of characterization methods, we connect electrochemical potential, thermodynamic stability, and electro-dissolution kinetics to the corrosion morphologies. Notably, under certain potential regimes, a micron-scale bicontinuous structure, characterized by a network of interconnected pores and ligaments riched with the composition of the more noble (MN) element, becomes prominent. At other potentials both MN and less noble (LN) elements dealloy but at different rates. The dealloying process consists of lattice and grain boundary diffusion of Cr to the metal/salt interface, interphase Cr oxidation, accompanied by surface diffusion of Ni to form interconnected ligaments. At higher potentials, the bicontinuous porous structure undergoes further surface coarsening. Concurrently, Cr(II), Cr(III), and Ni(II) begin to dissolve, with the dissolution of Ni occurring at a significantly slower rate. When solid-state transport of Cr is exceeded by the interfacial rates, dealloying depths are limited.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

An integrated approach to derive relative permeability from capillary pressure

Surface tension affects all aspects of fluid flow in porous media. Through measurements of surface tension interaction under multiphase conditions, a relative permeability curve can be determined. Relative permeability is a numerical description of the interaction between two or more fluids and the porous media. It is a critical parameter for various tools that characterize subsurface multiphase flow systems, such as numerical simulation for carbon sequestration, oil and gas development, and groundwater contamination remediation. Therefore, it is critical to get a good statistical distribution of relative permeability in the porous media under study. Empirical formula for determining relative permeability from capillary pressure are already well established but do not provide the needed flexibility that is required to match laboratory-derived relative permeability curves. By expanding the existing methods for calculating relative permeability from capillary pressure data, it is possible to create both two and three-phase relative permeability curves. Mercury intrusion capillary pressure (MICP) data from the Morrow 'B' Sandstone coupled with interfacial tension and contact angle measurements were used to create a suite of relative permeability curves. Furthermore, these curves were then calibrated to a small sample of existing laboratory curves to elucidate common fitting parameters for the formation that were then used to create relative permeability curves from MICP data that does not have an associated laboratory-measured relative permeability curve.

58 GEOSCIENCES↗

DOE OSTI2022

Capillary Pressure to Relative Permeability: Task 7.3.4 Relative Permeability Analysis Final Report

Surface tension affects all aspects of fluid flow in porous media. Through measurements of surface tension interaction under multiphase conditions, a relative permeability relationship can be determined. Relative permeability is a numerical description of the interplay between two or more fluids and the porous media they flow through. It is a critical parameter for various tools used to characterized subsurface multiphase flow systems, such as numerical simulation for oil and gas development, carbon sequestration, and groundwater contamination remediation. Therefore, it is critical to get a good statistic distribution of relative permeability in the porous media under study. Empirical relationships for determining relative permeability from capillary pressure are already well established but do not provide the needed flexibility required to match laboratory derive relative permeability relationships. By expanding the existing methods for calculating relative permeability from capillary pressure data, it is possible to create both two and three-phase relative permeability relationships. Existing laboratory-measured relative permeability data along with mercury intrusion capillary (MICP) data coupled with interfacial tension and contact angle measurements were used to determine the efficacy of this approach to relative permeability curve creation. The relative permeability relationships determined with this method were fit to existing laboratory data to elucidate common fitting parameters that were then used to create relative permeability relationships from MICP data that does not have an associated laboratory-measured relative permeability relationship.

58 GEOSCIENCES↗

DOE OSTI2020

Unusual electrical conductivity driven by localized stoichiometry modification at vertical epitaxial interfaces

Precise control of lattice mismatch accommodation and interfacial cation diffusion is critical to modulate correlated functionalities in epitaxial heterostructures, particularly when the interface composition is positioned near a compositional phase transition boundary. Here we select La 1-x Sr x MnO 3 (LSMO) as a prototype phase transition oxide and establish vertical epitaxial interfaces with NiO for exploring the strong interplay between strain accommodation, stoichiometry modification, and localized electron transport across the interface. It is found that localized stoichiometry modification overcomes the dead layer problem plaguing LSMO and leads to strongly directional conductivity, as manifested by a more than three orders of magnitude difference between out-of-plane and in-plane conductivity. Comprehensive atomic scale structural characterization and transport measurements reveal that this emerging behavior is created by a compositional change produced by preferential cation diffusion that pushes the LSMO phase transition from insulating into metallic within an ultrathin interface region. This study explores the nature of unusual electrical conductivity at vertical epitaxial interfaces and highlights the beneficial role of controllable cation diffusion that enables emerging functionalities for a broad range of potential applications such as memristors, spintronic devices, and novel nanoelectronic devices using strongly correlated materials.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Low-temperature formation of Ti2AlN during post-deposition annealing of reactive multilayer systems

M n+1 AXn-phase Ti 2 AlN thin-films were synthesized using reactive sputtering-based methods involving the deposition of single-layer TiAlN, and Ti/AlN and TiN/TiAl multilayers of various modulation periods at ambient temperature and subsequent annealing at elevated temperatures. Ex situ and in situ x-ray diffraction measurements were used to characterize the Ti 2 AlN formation temperature and phase fraction. During annealing, Ti/AlN multilayers yielded Ti 2 AlN at a significantly lower in situ temperature of 650 °C compared to TiN/TiAl multilayers or single-layer TiAlN (750 °C). The results suggest a reactive multilayer mechanism whereby distinct Ti and AlN layers react readily to release exothermic energy resulting in lower phase transition temperatures compared to TiN and TiAl layers or mixed TiAlN. With a modulation period of 5 nm, however, Ti/AlN multilayers yielded Ti 2 AlN at a higher temperature of 750 °C, indicating a disruption of the reactive multilayer mechanism due to a higher fraction of low-enthalpy interfacial TiAlN within the film.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Insight into pseudo-film-boiling in supercritical water under simplified interfacial conditions

The focus of this paper is the physics of supercritical water film boiling through the simulation of natural convection of supercritical water in a rectangular cavity. It has been widely believed that above a fluid's critical point, only one phase exists. However, recent research has indicated the existence of distinct gas-like and liquid-like regions separated by the Widom line, which is the locus of the maxima of the specific heat. Along the Widom line, density decreases sixfold, viscosity drops by a factor of two, while specific heat spikes by an order of magnitude. These variations, specifically in density and viscosity, produce a thick pseudo-interface and flow dynamics behavior akin to film-boiling, denoted here as pseudo-two-phase flow dynamics. When the cavity is heated from the bottom, a pseudo-film of gas-like fluid is formed at the heated wall, and the flow complexity evolves, characterized by the formation of multiple vortices. Results demonstrate the ability of modern conjugate heat transfer computational fluid dynamics to capture the pseudo two-phase regime, with the formation of a pseudo-film at the heated wall. Further, the boiling curve is studied, showing an increase in heat flux with an increase in the temperature differential between the wall and the pseudo-critical temperature. Furthermore, results also show a previously uncharacterized instability, where the convection cells in the cavity oscillate and can flip directions under certain conditions.

Computational fluid dynamics↗

DOE OSTI2022

Viscoelastic necking dynamics between attractive microgels

Hypothesis: Microgels can deform and interpenetrate and display colloid/polymer duality. The effective interaction of microgels in the collapsed state is governed by the interplay of polymer–solvent interfacial tension and bulk elasticity. A connecting neck is shown to mediate microgel interaction, but its temporal evolution has not been addressed. Here we hypothesize that the necking dynamics of attractive microgels exhibits liquid-like or solid-like behavior over different time and length scales. Experiments: We simulate the merging and pinching of attractive microgels with different crosslinking densities in explicit solvent using dissipative particle dynamics. The temporal coalescence dynamics of microgels is investigated and compared with simple liquid and polymeric droplets. We model the neck growth on long time scales using Maxwell model of polymer relaxation and compare the theoretical prediction with simulation data. The mechanical strength of the neck is characterized systematically via simulated pinch-off of microgels by steered molecular dynamics. Findings: We evidence a crossover in the coalescence dynamics reflecting the viscoelastic signature of microgels. In contrast to the common knowledge that viscoelastic materials respond elastically on short time scales, the early expansion of the microgel neck exhibits a linear behavior, similar to the viscous coalescence of liquid droplets. However, the late regime with arrested dynamics resembles sintering of solid particles. Through an analytical model relating microgel dynamics to neck growth, we show that the long-term behavior is governed by stress relaxation of the polymers in the neck region and predict an exponential decay in the rate of growth, which agrees favorably with the simulation. Different from coalescence, the thread thinning in microgel breakup primarily highlights its polymeric characteristics.

42 ENGINEERING↗

DOE OSTI2020

Nature of Terminating Hydroxyl Groups and Intercalating Water in Ti 3 C 2 T x MXenes: A Study by 1 H Solid-State NMR and DFT Calculations

Since the discovery of two-dimensional transition metal carbides, referred to as MXenes, research efforts targeted their applications in energy storage, as lithium-ion batteries and supercapacitors. This interest is attributable to MXenes’ large volumetric capacitance, high rate handling capability and stable cycling performance, which largely rely on surface chemistry provided by the terminating groups, such as -OH, -O, and -F. However, the atomic-scale characterization of these surface terminations challenges the diffraction methods. Solid-state (SS)NMR spectroscopy, especially 1 H SSNMR, is a promising approach for scrutinizing the surface terminations and the intercalated water in an atomistic-scale, yet only a few SSNMR studies in MXenes have been reported to date offering conflicting results and limited understanding of -OH terminations. Here, we used 1 H SSNMR experiments in concert with the DFT calculations of NMR parameters to identify multiple types of -OH groups, residing on the external and internal surfaces, in a commonly studied MXene, Ti 3 C 2 T x . The study also identifies bulk-like water trapped between the MXene flakes and interfacial water stranded on the surface. Lastly, two-dimensional 1 H -1 H correlation spectra elucidated the water-surface interactions and the mechanism of de-intercalation of water upon annealing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Tailoring compatibilization potential of maleic anhydride–grafted polypropylene by sequential rheochemical processing of polypropylene and polyamide 66 blends

Reactive compatibilization of immiscible polymer blends using a preferred compatibilizer leaves the following question: How much loading of a compatibilizer is good enough and what maximum properties can be achieved? A good understanding of the process can help solve the reutilization of mixed waste plastics. Here, the reactive compatibilization of polypropylene-graft-maleic anhydride (PP-g-MAH) on polypropylene/polyamide 66 (PP/PA66) blends is quantitatively assessed using thermorheological, microoptical, spectroscopic, and x-ray scattering-based characterization tools. The overall compositions of all PP(60%)/PA66(30%)/PP-g-MAH(10%) blends are kept constant while systematically controlling the degree of the chemical reaction by varying the sequential addition of PP-g-MAH to the melt mixture. The first feeding of PP-g-MAH (x%, 0 ≤ x ≤ 10) is conducted at 280°C and the second feeding of (10–x)% is at 200°C. During the first step, a larger amount of chemical activity is observed up to 4%–6% addition of PP-g-MAH. Furthermore, the constant chemical composition allows a systematic comparison of the compatibilizer-dependent thermal, rheological, morphological, and mechanical properties. With an increased degree of interfacial reaction, the size of dispersed PA66 domains decreases to register improved interfacial adhesion with the PP matrix, yielding enhanced Young's modulus and absolute failure strength of the isotropic matrix.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Orientational Ordering within Semiconducting Polymer Fibrils

Abstract Due to a general paucity of suitable characterization methods, the internal orientational ordering of polymer fibrils has rarely been measured despite its importance particularly for semi‐conducting polymers. An emerging tool with sensitivity to bond orientation is polarized resonant soft X‐ray scattering (P‐RSoXS). Here, P‐RSoXS reveals the molecular arrangement within fibrils (if type I or type II fibrils), the extent of orientation in the fibril crystal, and an explicit crystal‐amorphous interphase. Neat films as well as binary blends with a fullerene derivative are characterized for three different polymers, that are prototypical materials widely used in organic electronics applications. Anisotropic P‐RSoXS patterns reveal two different fibril types. Analysis of the q ‐dependence of the anisotropy from simulated and experimental scattering patterns reveal that neat polymer fibrillar systems likely comprise more than two phases, with the third phase in addition to crystal and amorphous likely being an interphase with distinct density and orientation. Intriguingly, the fibril type correlates to the H‐ or J‐aggregation signature in ultraviolet‐visible (UV–vis) spectroscopy, revealing insight into the fibril formation. Together, the results will open the door to develop more sophisticated structure‐function relationships between chemical design, fibril type, formation pathways and kinetics, interfacial ordering, and eventually device functions.

Mukherjee, Subhrangsu↗

DOE OSTI2021

Deactivation by Potassium Accumulation on a Pt/TiO 2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis

Biomass-derived feedstocks bring significant challenges to the longevity of the catalysts used for their conversion, and alkali metals, for example, K, in the feedstock have been widely ascribed as one of the important factors causing catalyst deactivation. To address this challenge, it is critical to understand the mechanism of catalyst deactivation caused by K accumulation to guide the improvement of catalysts and processes and the development of catalyst regeneration strategies. In this work, we report a deep understanding of the impact of K on a bifunctional Pt/TiO 2 catalyst, which is an efficient catalyst for the ex situ catalytic fast pyrolysis of biomass. We simulated the K-poisoning of Pt/TiO 2 catalysts by purposely loading different amounts of K (100-6000 ppm by weight) on the catalysts. A series of characterization approaches, including scanning transmission electron microscopy, Fourier transform infrared spectroscopy, and chemical titration, were combined with a kinetic assessment of multiple probe reactions to elucidate the mechanism of Pt/TiO 2 deactivation by K accumulation. At low K loadings (<800 ppm), K preferentially poisons the strong Lewis acid sites, leading to significantly reduced activity for acid-catalyzed alcohol dehydration. However, acetone condensation is less sensitive to the poisoning of strong Lewis acid sites. Reactions that occur on Pt sites or at the metal-support interface, including alkene hydrogenation, m-cresol hydrodeoxygenation (HDO), and CO oxidation, were not impacted. At high K loadings (>800 ppm), K starts to accumulate on the Pt-TiO 2 interfacial area, poisoning the interfacial active sites for HDO and CO oxidation reactions. We further found that the poisoning of the Pt/TiO 2 catalyst by K is reversible, and water washing can successfully remove the accumulated K and recover the activities for both alcohol dehydration and m-cresol HDO reactions.

09 BIOMASS FUELS↗

DOE OSTI2021

Effect of Surface Ionic Screening on Polarization Reversal and Phase Diagrams in Thin Antiferroelectric Films for Information and Energy Storage

Emergent behaviors in antiferroelectric thin films due to a coupling between surface electrochemistry and intrinsic polar instabilities are explored within the framework of the modified 2-4-6 Landau-Ginzburg-Devonshire (LGD) thermodynamic approach. By using phenomenological parameters of the LGD potential for a bulk antiferroelectric and a Stephenson-Highland (SH) approach, we study the role of surface ions with a charge density proportional to the relative partial oxygen pressure on the dipole states and their reversal mechanisms in antiferroelectric thin films. The combined LGDSH approach allows the boundaries of antiferroelectric, ferroelectriclike antiferroionic, and electretlike paraelectric states as a function of temperature, oxygen pressure, surface-ion formation energy and concentration, and film thickness to be delineated. This approach also allows the characterization of the polar and antipolar orderings dependence on the voltage applied to the antiferroelectric film, as well as the analysis of their static and dynamic hysteresis loops. Furthermore, the applications of the antiferroelectric films covered with a surface-ion layer for energy and information storage are explored and discussed.

25 ENERGY STORAGE↗

DOE OSTI2023

Using micro-XRF to characterize chloride ingress through cold joints in 3D printed concrete

Digital fabrication methods with concrete have been rapidly developing, with many problems related to component production and material control being solved in recent years. These processes produce inherently layered cementitious components that are anisotropic, and in many cases, produces a weak interface between layers, which are generally referred to as cold joints. While material strength at these interfaces has been well studied in recent years, durability has received less attention, even though cold joints can function as channels for aggressive agents, such as chlorides. This work presents a method using micro-X-ray fluorescence (μXRF) to image chloride ingress into layer interfaces of 3D printed fine-grained concrete specimens produced with varying layer deposition time intervals, and also compares it to neutron imaging of moisture uptake. The results show that cold joints formed after a 1 day time interval are highly susceptible to chloride ingress, and that curing conditions play a major role in how quickly interfacial transport can take place. The μXRF method is also shown to be useful for study of transport of chlorides in cold joints, due to its spatial resolution and direct analysis of an aggressive species of interest.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Microstructure prediction for Ti-22Al-25Nb in laser powder bed fusion

This work presents a physics-informed framework for predicting solidification morphology and defect susceptibility in additively manufactured Ti–22Al–25Nb across a broad processing space. The framework integrates solidification microstructure selection (SMS) analysis with a single-track defect-based printability map to establish a unified methodology linking processing parameters to both interfacial morphology and manufacturability. Thermal gradients G and solidification rates R are first computed using the Thermo-Calc Additive Manufacturing (TC-AM) module, a finite-interface-dissipation (FID) phase-field (PF) model coupled with CALPHAD method is then employed to systematically distinguish planar and dendritic regimes as functions of $G$ and $R$. By superimposing the printability map onto the morphology projections, a comprehensive process–structure framework is obtained. Across most processing conditions, the predicted microstructure is predominantly dendritic, while planar growth emerges only under selected laser power $P$ and scan speed $v$ combinations. In addition to morphology classification, the framework quantifies the dendritic area fraction and introduces a width-based morphology descriptor to characterize the spatial extent of planar/dendritic regions within the melt pool. It provides mechanistic insight into the interplay between solidification physics and defect formation, offering practical guidance for parameter selection and microstructural control in Ti–22Al–25Nb additive manufacturing (AM).

36 MATERIALS SCIENCE↗

DOE OSTI2025

Structural Evolution and Stability of Rh/TiO 2 Catalysts under CO 2 Hydrogenation Conditions: Influence of the Initial Rh Structure

Characterizing catalyst stability by identifying the predominant mechanisms, timescales and driving forces of catalyst reconstruction under relevant reaction conditions is necessary for the design and commercialization of new catalysts. Here, in this paper, we study Rh/TiO 2 catalysts under CO 2 hydrogenation conditions (773 K, 75% H 2 , 25% CO 2 ) at high conversion and utilize reactivity studies along with ex-situ and in-situ spectroscopy and microscopy to characterize changes in catalyst activity and structure as a function of time on stream and the initial catalyst structure. This is a prototypical catalyst for CO 2 hydrogenation where Rh structure and Rh-TiO 2 interactions have been proposed to explain reactivity, selectivity (between CO and CH 4 formation) and catalyst stability. The influence of the initial Rh structure (varying from Rh single atoms to Rh nanoparticles), support stability, regeneration and pretreatment(s), and the chemical potential(s) of the reaction environment on reaction selectivity and catalyst stability were explored. The product selectivity between CO and CH 4 was determined to be dependent on the relative fraction of Rh single atoms and Rh nanoparticle-TiO 2 interfacial sites under reaction conditions, each exhibiting distinct stability under prolonged time on stream. Surprisingly, Rh single atoms exhibited stability for the duration of 90 h reactivity measurements, even at high Rh density (≥ 1.8 Rh atoms/nm 2 ) on the support, while Rh nanoparticles sintered under reaction conditions. As a result, all catalysts exhibited increasing selectivity to CO with increasing time on stream (> 10 h). We conclude the distribution of Rh structures evolved over time under reaction conditions through three distinct reconstruction mechanisms (Rh particle fragmentation, Ostwald ripening, and particle migration and coalescence) that occurred on varying timescales. Catalyst stability on the ~90 h time scale was ultimately controlled by the initial Rh structure.

25 ENERGY STORAGE↗

DOE OSTI2025

Mesoporous Thin Film Architectures: Addressing Material Demands through Molecular Self-Assembly

Mesoporous thin films spark interest across a wide range of disciplines due to their tunable nanostructures, large internal surface areas, and strong compatibility with planar optical, electronic, and microfluidic devices. While attention in the porous materials community has shifted toward macroporous or disordered nanoporous systems, a resurgence in mesoporous thin film research is underway, driven by new molecular self-assembly methods, advanced materials chemistry, and improved characterization techniques. The integration of high-χN block copolymer design, kinetically persistent micelle templating, and postdeposition processing protocols now allows control over structural parameters such as pore size, wall thickness, porosity, and connectivity. These advances have overcome many of the thermodynamic and processing constraints that previously limited widespread adoption. Rather than serving only as high-surface-area supports, mesoporous thin films are engineered as active interfaces where responsive chemistries and nanoscale confinement act in tandem. Embedding switchable ligands, thermoresponsive polymers, redox mediators, or ion-selective groups directly within the pore walls enables real-time control over transport, optical, and electrochemical properties. These capabilities open up new directions in adaptive coatings, gated membranes, and fast-response biosensors. To further expand their functional scope, mesoporous films are integrated into hierarchical and multicomponent architectures. Techniques such as triblock terpolymer templating, crack-directed assembly, and nanoimprint lithography allow for control over spatial organization on the micron and submicron scale and pore system orientation. This enables programmable anisotropy, enhanced molecular diffusion, and wavelength-selective photonic behavior, essential for next-generation sensing, catalysis, and energy applications. Such structural and functional complexity requires equally sophisticated characterization. Multimodal and in situ techniques can track material dynamics under operational conditions. Recent progress includes extended-range ellipsometric porosimetry (EP) for hierarchical architectures, vacuum EP for interface energetics, time-resolved EP for diffusion kinetics, and correlative AFM-SAXS mapping. The introduction of advanced neutron-based spectroscopies, particularly quasielastic neutron scattering (QENS), promises to provide real-time access to ion transport dynamics and segmental motion under nanoscale confinement, offering a path toward deeper mechanistic understanding of structure-performance correlations in mesoporous systems. This Account reflects the technical advances made and the interdisciplinary collaborations that have shaped our collective vision. The particular dimensions of mesopores enable us to subtly tune interactions at the molecular, interfacial, and mesoscopic levels that permit us to harness nanoconfinement. What emerges is a versatile, modular platform capable of chemical gating, energy transduction, and sensing with a level of tunability unmatched by other porous materials. We highlight critical challenges including the need for more robust large-area processing, a deeper understanding of dynamic behavior under cycling, and better integration with device-level architectures. Our strategies support the transition of mesoporous thin films into active high-performance components in next-generation energy, environmental, and biomedical systems.

oxides↗

DOE OSTI2020

Beneficial Effect of Li 5 FeO 4 Lithium Source for Li-Ion Batteries with a Layered NMC Cathode and Si Anode

The energy density of lithium-ion batteries can be increased by replacing the traditional graphite anode with a high capacity silicon anode. However, volume changes and interfacial instabilities cause a large irreversible capacity and a continual loss of lithium during cycling, which lead to rapid capacity loss. In this work, we add Li 5 FeO 4 (LFO) to a LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC) cathode as a pre-lithiation additive, which increases the lithium inventory and extends the cycle life of Si-graphite/NMC full cells, and decreases the NMC particle degradation. LFO delivers a large 764 mAh g –1 LFO capacity below 4.7 V vs Li/Li + . By tuning the LFO content in Si-graphite/LFO-NMC full cells, we show higher capacity, improved retention, lower impedance, and superior rate performance compared to full cells without LFO. Post-test characterizations demonstrate that LFO inclusion in the cathode matrix leads to less NMC secondary particle segregation/cracking and a thinner surface reduced layer on the NMC particles. The beneficial effects of LFO endure after the lithium reserve has been exhausted, highlighting a lasting synergy between the lithium source and electrode active materials. This study introduces a new approach to simultaneously increase lithium inventory and reduce cathode degradation, and makes critical advances toward enabling Si anodes for lithium-ion batteries.

25 ENERGY STORAGE↗