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252 records · Page 14

High-temperature active oxidation of nanocrystalline silicon-carbide: A reactive force-field molecular dynamics study

Flexible woven SiC ceramics are prone to accelerated fiber embrittlement under high temperature oxidation in dynamic oxygen environments. The nanocrystalline structure of the constituent fibers impacts the reaction kinetics and phase transformations during active oxidation. However, fundamental understanding and quantification of grain boundary effects on oxidation behavior in nanocrystalline SiC remain elusive when temperatures exceed 1500 K. This study deploys large-scale molecular dynamics simulations with a reactive force-field to elucidate the complex roles of atomic oxygen reservoir conditions and grain size on oxidation kinetics and the nature of oxides produced in both monocrystalline and nanocrystalline 3C-SiC between 1100 K and 2000 K. The simulations with dynamically replenished oxygen provide good agreement with oxidation kinetics and activation energies for the monocrystalline Si(100) and C(100) orientations published in the available literature. This study reveals that, by contrast, nanocrystalline SiC samples exhibit two distinct oxidation kinetics with a transition point at 1500 K due to surface melting, which is supported by experimental evidence. The introduction of a grain-boundary network produces a two-fold decrease in oxidation activation energies compared to monocrystalline SiC below 1500 K. Above 1500 K, however, the activation energies rise substantially due to the formation of a liquid Si phase at the SiC/Si oxide interface. Further, it is shown that the stability of the interfacial liquid phase is promoted by incoherent grain boundaries in the crystalline SiC. These findings are important for the deployment of nanocrystalline SiC fibers in advanced thermal protection systems for high-temperature applications.

36 MATERIALS SCIENCE↗

A Versatile Approach to Stabilize Liquid–Liquid Interfaces using Surfactant Self-Assembly

Stabilizing liquid–liquid interfaces, whether between miscible or immiscible liquids, is crucial for a wide range of applications, including energy storage, microreactors, and biomimetic structures. Here, in this study, a versatile approach for stabilizing the water-oil interface is presented using the morphological transitions that occur during the self-assembly of anionic, cationic, and nonionic surfactants mixed with fatty acid oils. The morphological transitions underlying this approach are characterized and extensively studied through small-angle X-ray scattering (SAXS), rheometry, and microscopy techniques. Dissipative particle dynamics (DPD) as a simulation tool is adopted to investigate these morphological transitions both in the equilibrium ternary system as well as in the dynamic condition of the water-oil interface. Such a versatile strategy holds promise for enhancing applications such as liquid-in-liquid 3D printing. Moreover, it has the potential to revolutionize a wide range of fields where stabilizing liquid–liquid interfaces not only offers unprecedented opportunities for fine-tuning nanostructural morphologies but also imparts interesting practical features to the resulting liquid shapes. These features include perfusion capabilities, self-healing, and porosity, which could have significant implications for various industries.

36 MATERIALS SCIENCE↗

Understanding Self-Assembly and the Stabilization of Liquid/Liquid Interfaces: The Importance of Ligand Tail Branching and Oil-Phase Solvation

Organophosphorus-based ligands represent a versatile set of solvent extraction reagents whose chemical makeup plays an important role in extraction mechanism. We hypothesize that the branching of the extractant hydrophobic tail and its oil-phase solvation affect the liquid/liquid interfacial structure. Understanding the structure mediated adsorption and interfacial ordering becomes key in designing ligands with enhanced selectivity and efficiency for targeted extractions. We employed vibrational sum frequency generation spectroscopy and interfacial tension measurements to extract thermodynamic adsorption energies, map interfacial ordering, and rationalize disparate behaviors of model di-(2-ethylhexyl) phosphoric acid and dioctyl phosphoric acid ligands at the hexadecane water interface. With increased surface loading, ligands with branched hydrophobic tails formed stable interfaces at much lower concentrations than those observed for ligands with linear alkyl tails. The lack of an oil phase and associated solvation results in markedly different interfacial properties, and thus measurements made at air/liquid surfaces cannot be assumed to correlate with the processes occurring at buried liquid/liquid interfaces. Here, we attribute these differences in the surface mediated self-assembly to key variations in hydrophobic interactions and tail solvation taking place in the oil phase demonstrating that interactions in both the polar and nonpolar phases are essential to understand self-assembly and function.

36 MATERIALS SCIENCE↗

High-Pressure Lightweight Thrusters

Returning samples of Martian soil and rock to Earth is of great interest to scientists. There were numerous studies to evaluate Mars Sample Return (MSR) mission architectures, technology needs, development plans, and requirements. The largest propulsion risk element of the MSR mission is the Mars Ascent Vehicle (MAV). Along with the baseline solid-propellant vehicle, liquid propellants have been considered. Similar requirements apply to other lander ascent engines and reaction control systems. The performance of current state-ofthe- art liquid propellant engines can be significantly improved by increasing both combustion temperature and pressure. Pump-fed propulsion is suggested for a single-stage bipropellant MAV. Achieving a 90-percent stage propellant fraction is thought to be possible on a 100-kg scale, including sufficient thrust for lifting off Mars. To increase the performance of storable bipropellant rocket engines, a high-pressure, lightweight combustion chamber was designed. Iridium liner electrodeposition was investigated on complex-shaped thrust chamber mandrels. Dense, uniform iridium liners were produced on chamber and cylindrical mandrels. Carbon/carbon composite (C/C) structures were braided over iridium-lined mandrels and densified by chemical vapor infiltration. Niobium deposition was evaluated for forming a metallic attachment flange on the carbon/ carbon structure. The new thrust chamber was designed to exceed state-of-the-art performance, and was manufactured with an 83-percent weight savings. High-performance C/Cs possess a unique set of properties that make them desirable materials for high-temperature structures used in rocket propulsion components, hypersonic vehicles, and aircraft brakes. In particular, more attention is focused on 3D braided C/Cs due to their mesh-work structure. Research on the properties of C/Cs has shown that the strength of composites is strongly affected by the fiber-matrix interfacial bonding, and that weakening interface realizes pseudo-plastic behavior with significant increase in the tensile strength. The investigation of high-temperature strength of C/Cs under high-rate heating (critical for thrust chambers) shows that tensile and compression strength increases from 70 MPa at room temperature to 110 MPa at 1,773 K, and up to 125 MPa at 2,473 K. Despite these unique properties, the use of C/Cs is limited by its high oxidation rate at elevated temperatures. Lining carbon/carbon chambers with a thin layer of iridium or iridium and rhenium is an innovative way to use proven refractory metals and provide the oxidation barrier necessary to enable the use of carbon/ carbon composites. Due to the lower density of C/Cs as compared to SiC/SiC composites, an iridium liner can be added to the C/C structure and still be below the overall thruster weight. Weight calculations show that C/C, C/C with 50 microns of Ir, and C/C with 100 microns of Ir are of less weight than alternative materials for the same construction.

Holmes, Richard↗

A versatile approach to stabilize liquid-liquid interfaces using surfactant self-assembly

Stabilizing liquid–liquid interfaces, whether between miscible or immiscible liquids, is crucial for a wide range of applications, including energy storage, microreactors, and biomimetic structures. In this study, a versatile approach for stabilizing the water-oil interface is presented using the morphological transitions that occur during the self-assembly of anionic, cationic, and nonionic surfactants mixed with fatty acid oils. The morphological transitions underlying this approach are characterized and extensively studied through small-angle X-ray scattering (SAXS), rheometry, and microscopy techniques. Dissipative particle dynamics (DPD) as a simulation tool is adopted to investigate these morphological transitions both in the equilibrium ternary system as well as in the dynamic condition of the water-oil interface. Such a versatile strategy holds promise for enhancing applications such as liquid-in-liquid 3D printing. Moreover, it has the potential to revolutionize a wide range of fields where stabilizing liquid–liquid interfaces not only offers unprecedented opportunities for fine-tuning nanostructural morphologies but also imparts interesting practical features to the resulting liquid shapes. These features include perfusion capabilities, self-healing, and porosity, which could have significant implications for various industries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chain Dynamics in Magnetorheological Suspensions

Magnetorheological (MR) suspensions are composed of colloidal particles which acquire dipole moments when subjected to an external magnetic field. At sufficient field strengths and concentrations, the dipolar particles rapidly aggregate to form long chains. Subsequent lateral cross-linking of the dipolar chains is responsible for a rapid liquid-to-solid-like rheological transition. The unique, magnetically-activated rheological properties of MR suspensions make them ideal for interfacing mechanical systems to electronic controls. Additionally, the ability to experimentally probe colloidal suspensions interacting through tunable anisotropic potentials is of fundamental interest. Our current experimental work has focused on understanding the fluctuations of dipolar chains. It has been proposed by Halsey and Toor (HT) that the strong Landau-Peierls thermal fluctuations of dipolar chains could be responsible for long-range attractions between chains. Such interactions will govern the long-time relaxation of MR suspensions. We have synthesized monodisperse neutrally buoyant MR suspensions by density matching stabilized ferrofluid emulsion droplets with D2O. This allows us to probe the dynamics of the dipolar chains using light scattering without gravitational, interfacial, and polydispersity effects to resolve the short-wavelength dynamics of the dipolar chains. We used diffusing wave spectroscopy to measure these dynamics. The particle displacements at short times that show an independence to the field strength, but at long times exhibit a constrained, sub-diffusive motion that slows as the dipole strength is increased. The experiments are in good qualitative agreement with Brownian dynamics simulations of dipolar chains. Although there have been several important and detailed studies of the structure and interactions in MR suspensions, there has not been conclusive evidence that supports or contradicts the HT model prediction that long-range interactions exist between fluctuating chains of dipolar particles. Resolving this issue would contribute greatly to the understanding of these interesting and important materials. We have begun to test the predictions of the HT model by both examining the dynamics of individual chains and by measuring the forces between dipolar chains directly to accurately and quantitatively assess the interactions that they experience. To do so, we employ optical trapping techniques and video-microscopy to manipulate and observe our samples on the microscopic level. With these techniques, it is possible to observe chains that are fluctuating freely in three-dimensions, independent of interfacial effects. More importantly, we are able to controllably observe the interactions of two chains at various separations to measure the force-distance profile. The techniques also allow us to study the mechanical properties of individual chains and chain clusters. Our work to this point has focused on reversibly-formed dipolar chains due to field induced dipoles where the combination of this chaining, the dipolar forces, and the hydrodynamic interactions that dictate the rheology of the suspensions. One can envision, however, many situations where optical, electronic, or rheological behavior may be optimized with magneto-responsive anisotropic particles. Chains of polarizable particles may have the best properties as they can coil and flex in the absence of a field and stiffen and orient when a field is applied. We have recently demonstrated a synthesis of stable, permanent paramagnetic chains by both covalently and physically linking paramagnetic colloidal particles. The method employed allows us to create monodisperse chains of controlled length. We observed the stability, field-alignment, and rigidity of this new class of materials. The chains may exhibit unique rheological properties in an applied magnetic field over isotropic suspensions of paramagnetic particles. They are also useful rheological models as bead-spring systems. These chains form the basis for our current experiments with optical traps.

Gast, A. P.↗

Analysis of Laminar Convective Heat Transfer Over Structured Non-Wetting Surfaces

Structured non-wetting surfaces provide alternating no-slip and partial slip boundary conditions to the fluid flow which, in turn, affects the convective heat transfer performance over the surfaces. In this work, an analytical model is developed for the interfacial Nusselt number, the overall Nusselt number and a thermal hydraulic performance factor for fluid flow in a cylinder patterned with structured non-wetting surfaces, for the two cases of uniform wall heat flux and uniform wall temperature. In addition, by considering the stability of the Cassie state of wettability and its transition to the Wenzel state for flow over superhydrophobic surfaces, the present model overcomes certain limitations of the previously reported studies in the literature. Based on the analytical formulations and the stability constraints, the present paper provides optimum design maps for tailoring structured non-wetting surfaces for maximizing convective heat transfer and the combined thermal-hydraulic performance in applications. Use of the design maps on example cases is also discussed. It is shown that the use of structured non-wetting surfaces is most effective for low Reynolds numbers and/or small cylinder radius.

42 ENGINEERING↗

Interfacial Fabrication of Supramolecular Polymer Networks Using Mussel-Inspired Catechol–Iron Complexes

The liquid–liquid interface provides a promising platform to construct supramolecular polymers and materials with advanced functions. However, supramolecular polymerization at the interface usually requires monomers with different or even orthogonal solubilities, which significantly limit the number of usable monomers. Here, in this work, we report a new strategy to construct supramolecular polymer networks at the oil–water interface using a water-soluble catechol–iron complex and an oil-soluble diend-functionalized polymer. Owing to the dynamic catechol–iron coordination bond and imine bond, the resulting supramolecular polymer networks demonstrate excellent dynamic features and responsiveness to different stimuli including the pH, redox, competing ligands, and temperature. With a supramolecular polymer network serving as a building block, emulsions and 2D films can be generated that have potential applications in encapsulation, release, and molecular separation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observations of grain-boundary phase transformations in an elemental metal

The theory of grain boundary (the interface between crystallites, GB) structure has a long history 1 and the concept of GBs undergoing phase transformations was proposed 50 years ago 2,3 . The underlying assumption was that multiple stable and metastable states exist for different GB orientations 4,5,6 . The terminology ‘complexion’ was recently proposed to distinguish between interfacial states that differ in any equilibrium thermodynamic property 7 . Different types of complexion and transitions between complexions have been characterized, mostly in binary or multicomponent systems 8,9,10,11,12,13,14,15,16,17,18,19 . Simulations have provided insight into the phase behaviour of interfaces and shown that GB transitions can occur in many material systems 20,21,22,23,24 . However, the direct experimental observation and transformation kinetics of GBs in an elemental metal have remained elusive. In this work we demonstrate atomic-scale GB phase coexistence and transformations at symmetric and asymmetric $[11\bar{1}]$ tilt GBs in elemental copper. Atomic-resolution imaging reveals the coexistence of two different structures at Σ19b GBs (where Σ19 is the density of coincident sites and b is a GB variant), in agreement with evolutionary GB structure search and clustering analysis 21,25,26 . We also use finite-temperature molecular dynamics simulations to explore the coexistence and transformation kinetics of these GB phases. Our results demonstrate how GB phases can be kinetically trapped, enabling atomic-scale room-temperature observations. Our work paves the way for atomic-scale in situ studies of metallic GB phase transformations, which were previously detected only indirectly 9,15,27,28,29 , through their influence on abnormal grain growth, non-Arrhenius-type diffusion or liquid metal embrittlement.

36 MATERIALS SCIENCE↗

Impact Ice Adhesion at NASA Glenn: Current Experimental Methods and Supporting Measurements

When examining the literature on the adhesion strength of impact ice, there have been a wide range of methodologies tried to measure the required stresses to induce interfacial delamination. Utilizing the Icing Research Tunnel at the NASA Glenn Research Center to generate the impact ice required for this work, several different mechanical tests have been and are being developed to determine the stresses along the interface between ice and coupon. This set of tests includes the technical mature modified lap joint test which has been used to conduct ice adhesion studies through a wide sweep of icing conditions. To conduct in situ ice adhesion measurements inside of the Icing Research Tunnel, several new experiments are currently being developed to make ice adhesion measurements during and immediately after ice accretion. In addition to these experimental methods, several supporting measurement techniques have been developed to allow for a better understanding on the influence of icing cloud conditions on the mechanical behavior of impact ice. Digital image correlation has been successfully implemented to augment the data generated by the modified lap joint test with full field surface displacement and strain measurements which allow for insight into the deformation processes present during a test. Both optical microscopy of impact ice samples along with ice replication techniques have been used to study the grain structure of the impact ice. This has led to a deeper understanding of the results from the modified lap joint method and how the structure of impact ice changes as it is accreted during an icing spray. The freezing process of impact ice generated by supercooled liquid water is not a volume conserving process, which leads to the presence of residual strains along the interface between ice and substrate. These strains have been observed using both a simplified flat geometry and a representative airfoil. The data gathered by these experimental adhesion methods and supporting measurements allows for a comprehensive understanding on the behavior of impact ice which will be critical to the development of future ice shedding models.

Ice Adhesion↗

Impact Ice Adhesion at NASA Glenn: Current Experimental Methods and Supporting Measurements

When examining the literature on the adhesion strength of impact ice, there have been a wide range of methodologies tried to measure the required stresses to induce interfacial delamination. Utilizing the Icing Research Tunnel at the NASA Glenn Research Center to generate the impact ice required for this work, several different mechanical tests have been and are being developed to determine the stresses along the interface between ice and coupon. This set of tests includes the technical mature modified lap joint test which has been used to conduct ice adhesion studies through a wide sweep of icing conditions. To conduct in situ ice adhesion measurements inside of the Icing Research Tunnel, several new experiments are currently being developed to make ice adhesion measurements during and immediately after ice accretion. In addition to these experimental methods, several supporting measurement techniques have been developed to allow for a better understanding on the influence of icing cloud conditions on the mechanical behavior of impact ice. Digital image correlation has been successfully implemented to augment the data generated by the modified lap joint test with full field surface displacement and strain measurements which allow for insight into the deformation processes present during a test. Both optical microscopy of impact ice samples along with ice replication techniques have been used to study the grain structure of the impact ice. This has led to a deeper understanding of the results from the modified lap join method and how the structure of impact ice changes as it is accreted during an icing spray. The freezing process of impact ice generated by supercooled liquid water is not a volume conserving process, which leads to the presence of residual strains along the interface between ice and substrate. These strains have been observed using both a simplified flat geometry and a representative airfoil. The data gathered by these experimental adhesion methods and supporting measurements allows for a compressive understanding on the behavior of impact ice which will be critical to the development of future ice shedding models.

Ice Adhesion↗

Liquid Interfacial Electron Microscopy Identifies Nanogalvanic Corrosion in Pearlitic Steel

The nanoscale mechanisms of localized corrosion in low carbon steels have remained elusive due to the complexity of studying the degradative material behavior at nanoscale solid-liquid interfaces. We identified various steps in the nanogalvanic corrosion processes using in-situ liquid-cell scanning transmission electron microscopy (STEM) using a microfluidic holder by Hummingbird Scientific. Initial work, performed at low magnification, identified the initiation point on a 1018 low-carbon steel surface. This initiation point was determined to be a triple junction of two ferrite grains bridging a cementite grain in contact with a baseline electrolyte of 6 uM CO2 dissolved in a buffered (2.78 uM Na2SO4) aqueous solution, pH 6.1. The pre-etched low-carbon steel surface was prepared using focused ion beam lift-out procedures to extract a cross-section of the low-carbon steel surface, which then was thinned to about 150 nm and transferred to a SiN membrane microfluidic window. The transfer was made using a lift-out needle to attach the low-carbon steel lamella to the corner of the SiN window, and then Pt/C deposition held the lamella in contact with the window while it was released from the lift out needle. To identify the triple point on the low carbon steel lamella, prior to attachment on the SiN window, the sample was characterized for compositional variations with energy dispersive x-ray spectroscopy mapping, grain orientation and phase mapping with precession electron diffraction, and thickness mapping with energy filtered transmission electron microscopy. This pre-characterization prior to the in-situ experiment provided a map of the multiphase and multigrain structure, where the in-situ liquid cell imaging provided a clear understanding of the initiation point on the sample. These data were cross-correlated to paint a holistic picture of the triple junction site, enabling low electron-fluence in-situ snapshot imaging to avoid dominating the native corrosion reactions with effects from the incident electron beam. This initial result identified that localized, nanogalvanic corrosion at the phase interface was the dominant corrosion process in the low-carbon steel, so we next targeted the observation of an array of these nanogalvanic features phase boundaries in a pearlite grain. Near-surface ferrite/cementite phase interfaces that typify pearlitic low-carbon steel were extracted, pre-characterized, and imaged for the in-situ corrosion processes. The sample was a cross-section from a pearlite grain, with alternating ferrite and cementite grains that extended microns down from the pre-etched low-carbon steel pipe surface. After contact with a buffered aqueous solution, the phase boundaries between the ferrite and cementite began to dissolve, with observable material loss and thickness changes in the dark-field and bright-field STEM images. Within minutes, the corrosion front proceeded deeper into the material, claiming a thin layer of ferrite around all exposed phase boundaries before progressing laterally into the ferrite matrix, converting the ferrite to corrosion product normal to each buried cementite grain. Formation of the corrosion product causes a volumetric expansion, creating a lateral wedging force that mechanically ejects the cementite grains from their grooves and leaves behind percolation channels into the steel substructure. Rapid and deleterious, this nanogalvanic corrosion pathway represents an important target for understanding and preventing run-away degradation in this common building material. Observation of this corrosion mechanism was enabled by the combination of pre-characterization using standard structural, grain, and compositional analysis in the TEM, which provides maps for understanding the reaction propagation captured in low-dose, in-situ, liquid-cell STEM.

corrosion↗

Magnetic Response of Excitons and Excitonic Complexes in Defective Hexyl Ammonium Lead Iodide Self-Assembled Quantum Wells

Correlating the magnetic behavior of low-dimensional semiconductors with the chemistry used to form these excitonic materials remains crucial to the development of devices applied to quantum technologies. In this study, we apply large magnetic fields during the collection of low-temperature photoluminescence (PL) to assess the magnetic properties of excitons in hexyl ammonium lead iodide (HA 2 PbI 4 ) self-assembled quantum wells (SAQWs) formed at liquid−liquid interfaces. The effect of incident laser power and temperature was used to assign lower energy features in these samples’ PL spectra to both excitons trapped at defect sites and trions. Measured peaks shifts allow us to estimate coupling between the applied magnetic fields and the charged defect excitons. Our conclusions are supported by density functional theory calculations on supercells of the proposed defective HA 2 PbI 4 SAQW structure. Additionally, we find an anomalous magnetic response from trion states that resembles the behavior of interacting excitonic complexes in similar, quantum-confined materials at low temperatures. These results highlight the crucial role that chemical conditions can play in the magnetic response of 2D semiconductors applied in quantum technologies.

defect chemistry↗

VTO_2021_APR_LLNL_Ye

Traditional batteries are composed of two-dimensional films that are stacked and/or rolled. Thin film batteries display high power density while their thick film counterparts show good energy density, but it has proven difficult to concurrently achieve both within these planar form factors. In addition, conventional Li-ion batteries based on liquid organic electrolytes or gel polymer electrolytes have raised severe safety concerns due to the intrinsic flammable properties of the organic electrolytes. They are also not ideal for the use of high energy density metallic lithium (Li) anodes due to Li dendrite growth, or sulfur cathodes due to shuttling effects that result in fast capacity fade. There is an urgent need to develop safe, high-performance solid-state batteries (SSBs) with advanced electrolyte and separator technologies. Although in recent years a series of superionic conductors have been developed for electrolytes and separators, their performance does not satisfy demanding criteria due to large impedance from poor solid electrolyte-electrode contact and questionable electrochemical and mechanical stability. Unlike the well-established roll-to-roll fabrication of conventional Li-ion batteries, the processing of SSBs is unique due to the brittleness of solid-state electrolytes (SSEs). The commercially available or lab-developed SSE discs are usually very thick (hundreds of micrometers to millimeters) to overcome their brittle nature, which unfortunately increases the cell impedance and accounts for the majority of the overall cell weight and volume, leading to dramatically decreased power and energy densities. In this project, we will investigate 3D printing techniques to overcome safety, fabrication, mechanical, and electrochemical issues in SSBs. 3D printing builds complex structures in a layer-by-layer fashion, which allows rapid production of hierarchical architectures, gradient and multi-material structures, and multi-component assemblies. 3D printing is an emerging area that could fundamentally transform energy storage devices. For example, 3D printing can produce batteries with arbitrary form factors to fit a product’s specific volume requirements and can create interwoven electrode arrangements over a wide range of length scales to improve transport and increase power density for a given energy density. For SSBs, 3D printing may dramatically reduce the separator thickness from ~1 mm (by hydraulic pressing) to tens of micrometers or less. In addition, the interfacial contact area between the electrolyte and the electrode may be increased via 3D interdigitated designs. Hence, we expect a significant reduction of the overall cell impedance and enhancement of both energy and power densities of SSBs by harnessing an array of 3D printing technologies being developed at Lawrence Livermore National Laboratory (LLNL).

25 ENERGY STORAGE↗

A First Principles Approach to Spectral Phonon Transport in Heterostructures

Understanding thermal transport across interfaces which give rise to a thermal resistance (also known as Kapitza resistance) is a critical issue affecting the development of nanotechnologies. Much modern and emergent nanotechnology consist of adjacent materials, and phonon mediated heat transfer governs thermal behavior across internal interfaces in these devices. The physics of thermal transport in solids are governed both by phenomena occurring at the atomic scale and interactions with the material's microstructure. The forecasting of fundamental quantities such as temperature, heat flux and thermal conductivity typically employs the semi-classical Boltzmann transport equation to predict the macroscopic behavior of materials in terms of the microscopic dynamics of its heat carriers. Kapitza resistance was first discovered in liquid helium experiments and has led to a fundamental research thrust in micro and nano-scale heat transport, the behavior of thermal carriers across internal interfaces. Thermal interfacial resistance (TIR) is a widely studied phenomenon, first engaged by Swartz and Pohl through their development of the acoustic and diffuse mismatch methods, then continued through myriad efforts with varying methods and approaches in an attempt to resolve carrier behavior at thermal interfaces. Many of the fundamental approaches to TIR have been at the nanoscale, and research is conducted with molecular dynamics (MD) and density functional theory (DFT) methods. The limitations of these methods is system size; atomistic methods tend to be limited to system sizes of 100,000 atoms or less. Larger length-scale methods have also been pursued, based on the principles of acoustic or diffuse mismatch, but not all include simulation of TIR using a full phonon band spectrum, or temperature dependent methods. Our approach to enabling phonon transport in layered materials draws upon our previous work of demonstrating spectrally coupled phonon transport in homogeneous and heterogeneous materials. We use a semi-analytical approach in which the Bose-Einstein (B-E) statistics set the strength of the phonon radiance in a frequency group, but the B-E statistics are informed with information from the transport system. The B-E statistics in a single frequency group feels the influence of all the groups through the spatial temperature. We also include a new field term which is an indicator of the amount of non-equilibrium behavior of the phonon spectrum---this is added to the phonon source term in all groups to ensure closure and conservation of energy, as the phonon groups in the transport system and the analytical systems are coupled. This work builds upon our previous approach by adding a phonon coupling term at an internal interface, using the principles of the DMM through transmission and reflection coefficients. In this work, the coefficients are determined through computing a common temperature at the interface, influenced by the phonon band structure of both materials, in effect, providing mixing between the two material systems and using the common temperature to set the strength of the phonon radiance at the boundaries on either side of the interface. Our approach uses material properties computed along various crystallographic orientations, and while some isotropy is built into the interface condition, the material properties weight the phonon distributions in the proper crystalline direction. Greater resolution of phonon behavior in proximity to an interface, and more accurate predictions of TIR are obtained. While it is true the assumption of diffuse mismatch can yield inconsistent results compared to experiment especially at low temperatures, this work focuses on room temperature and beyond effects, for future applications in nuclear fuel, or thermoelectric devices; a modified mismatch approach may be feasible if applied properly. Additionally, our methods focus on bridging mesoscale to engineering scale

36 MATERIALS SCIENCE↗

Thermally Driven Interfacial Degradation between Li 7 La 3 Zr 2 O 12 Electrolyte and LiNi 0.6 Mn 0.2 Co 0.2 O 2 Cathode

Solid-state batteries offer higher energy density and enhanced safety compared to the present lithium-ion batteries using liquid electrolytes. A challenge to implement them is the high resistances, especially at the solid electrolyte interface with the cathode. Sintering at elevated temperature is needed in order to get good contact between the ceramic solid electrolyte and oxide cathodes and thus to reduce contact resistances. Many solid electrolyte and cathode materials react to form secondary phases. It is necessary to find out which phases arise as a result of interface sintering and evaluate their effect on electrochemical properties. Herein, we assessed the interfacial reactions between LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) and Li 7 La 3 Zr 2 O 12 (LLZO) as a function of temperature in air. We prepared model systems by depositing thin-film NMC622 cathode layers on LLZO pellets. The thin-film cathode approach enabled us to use interface-sensitive techniques such as X-ray absorption spectroscopy in the near-edge as well as the extended regimes and identify the onset of detrimental reactions. We found that the Ni and Co chemical environments change already at moderate temperatures, on-setting from 500 °C and becoming especially prominent at 700 °C. By analyzing spectroscopy results along with X-ray diffraction, we identified Li 2 CO 3 , La 2 Zr 2 O 7 , and La(Ni,Co)O 3 as the secondary phases that formed at 700 °C. The interfacial resistance for Li transfer, measured by electrochemical impedance spectroscopy, increases significantly upon the onset and evolution of the detected interface chemistry. Our findings suggest that limiting the bonding temperature and avoiding CO 2 in the sintering environment can help to remedy the interfacial degradation.

36 MATERIALS SCIENCE↗

SISGR: Chemomechanics of Far-From-Equilibrium Interfaces (COFFEI)

Portable, reliable, and deployable devices for energy storage and conversion require fundamental changes in design of solid-state composites comprising ceramics and metals. These materials comprise the electrodes and electrolytes of next-generation solid-oxide fuel cells and all solid-state batteries, forming solid-state functional composites. The advent of solid-state batteries – which replace liquid electrolytes with solid electrolytes capable of lithium ion transport for reliable energy storage in portable batteries – and the increased demand space for all solid-state fuel cells capable of oxygen reduction at intermediate temperatures remain important challenges for improved material stability and decreased system cost. However, little is understood about three fundamental facets of materials that enable such solid-state energy applications. First, how do such materials deform, fracture, or delaminate under operando conditions? Second, how does such mechanical deformation limit or facilitate electronic and ionic transport within and across such material interfaces? Third, how we can predictably design interface-rich composites to engineer both structural and electrochemical stability? This COFFEI Group comprised expertise from Materials Science & Engineering and Nuclear Science & Engineering to integrate unique in situ experiments, simulations, and fabricated interfaces that address these fundamental questions in solid-state interfaces of nanoscale composites that will guide solid-state electrochemistry, transport kinetics, and mechanical deformation for nonstoichiometric materials that enable such applications. In particular, we built on COFFEI’s understanding of chemomechanical coupling among defect concentrations, ionic transport, electron transport, and stored elastic energy that is particularly acute in the far-from-equilibrium conditions typical of energy device applications. By tailoring our focus to solid-state interfaces, we addressed these important issues by (a) developing and applying advanced in situ and ex situ characterization tools to characterize model materials and interfaces synthesized with molecular-level control, under both laboratory-controlled and extreme environments representative of energy device operation; and (b) employing computational modeling and simulation frameworks to predict transport mechanisms, reactivity and stability of these model materials and interfaces under significant chemical strains typical of energy device operation. Recent progress provided insights to additional materials systems and electrochemomechanical fatigue and fracture that were not fully envisioned when the program was initiated. Specifically, in the final three years of COFFEI we pursued two integrated thrusts, with complementary focus. Thrust I focused on failure-resistant electrochemomechanical composites, while Thrust II focused on strain-modulated conductivity and reactivity across interfaces. In contrast to our initial COFFEI focus, these thrusts concentrated wholly on solid-state material interfacial interactions and included greater integration of multiscale visualization including in situ electron microscopy of strained structures/interactions and mesoscale simulations. Successful development of functionally superior and long-lived battery and fuel cell systems and stress adaptable oxides requires a deeper, fundamental understanding of the coupling among the historically important subfields of solid-state electrochemistry, transport kinetics, and mechanical deformation for nonstoichiometric metal oxide electrodes. In this program, the understanding and the application of chemomechanical coupling of defect concentrations, ionic transport, electro-catalytic activity and stored elastic energy, particularly acute in the far-from-equilibrium conditions typical of energy device applications, are being refined and implications for device operation clarified, including for miniaturized solid-state batteries and fuel cells.

36 MATERIALS SCIENCE↗

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗