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At least 631 records · Page 35

Instabilities and phase transitions in architected metamaterials: a gradient-enhanced continuum approach

Architected metamaterials such as foams and lattices exhibit a wide range of properties governed by microstructural instabilities and emerging phase transitions. Their macroscopic response–including energy dissipation during impact, large recoverable deformations, morphing between configurations, and auxetic behavior–remains difficult to capture with conventional continuum models, which often rely on discrete approaches that limit scalability. In this work, we propose a nonlocal continuum formulation that captures both stable and unstable responses of elastic architected metamaterials. The framework extends anisotropic hyperelasticity by introducing nonlocal variables and internal length scales reflective of microstructural features. Local polyconvex free-energy models are systematically augmented with two families of non-(poly)convex energies, enabling both metastable and bistable responses. Implementation in a finite element framework enables solution using a hybrid monolithic–staggered strategy. Simulations capture densification fronts, forward and reverse transitions, hysteresis loops, imperfection sensitivity, and globally coordinated auxetic modes. Overall, this framework provides a robust foundation for accelerated modeling of instability-driven phenomena in architected metamaterials, while enabling extensions to anisotropic, dissipative, and active systems as well as integration with data-driven and machine learning approaches.

42 ENGINEERING↗

Slow spin dynamics in the hyperhoneycomb lattice [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 revealed by H 1 NMR studies

We report the results of magnetic susceptibility χ and H 1 nuclear magnetic resonance (NMR) measurements on a three-dimensional hyperhoneycomb lattice compound [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 (CCCO). The average value of the antiferromagnetic (AFM) exchange coupling between the Cu 2 + ( S = 1 / 2 ) spins was determined to be J ~ 50 K from the χ measurements. No long-range magnetic ordering has been observed down to T = 50 mK, although NMR lines become slightly broader at low temperatures below 1 K. The broadening of the NMR spectrum observed below 1 K reveals that the Cu spin moments remain at this temperature, suggesting a non-spin-singlet ground state. The temperature and magnetic field dependence of 1 / T 1 at temperatures above 20 K is well explained by paramagnetic thermal spin fluctuations where the fluctuation frequency of Cu 2 + spins is higher than the NMR frequency of the order of megahertz. However, a clear signature of the slowing down of the Cu 2 + spin fluctuations was observed at low temperatures where 1 / T 1 shows a thermally activated behavior. The magnetic field dependence of the magnitude of the spin excitation gap suggests that the magnetic behaviors of CCCO are characterized as an AFM chain at low temperatures.

1-dimensional systems↗

Atomic Three-Dimensional Investigations of Pd Nanocatalysts for Acetylene Semi-hydrogenation

Deciphering the three-dimensional (3D) insight into nanocatalyst surfaces at the atomic level is crucial to understanding catalytic reaction mechanisms and developing high-performance catalysts. Nevertheless, better understanding the inherent insufficiency of a long-range ordered lattice in nanocatalysts is a big challenge. Here, in this work, we report the local structure of Pd nanocatalysts, which is beneficial for demonstrating the shape-structure-adsorption relationship in acetylene hydrogenation. The 5.27 nm spherical Pd catalyst (Pd sph ) shows an ethylene selectivity of 88% at complete acetylene conversion, which is much higher than those of the Pd octahedron and Pd cube and superior to other reported monometallic Pd nanocatalysts so far. By virtue of the local structure revelation combined with the atomic pair distribution function (PDF) and reverse Monte Carlo (RMC) simulation, the atomic surface distribution of the unique compressed strain of Pd-Pd pairs in Pd sph was revealed. Density functional theory calculations verified the obvious weakening of the ethylene adsorption energy on account of the surface strain of Pd sph . It is the main factor to avoid the over-hydrogenation of acetylene. The present work, entailing shape-induced surface strain manipulation and atomic 3D insight, opens a new path to understand and optimize chemical activity and selectivity in the heterogeneous catalysis process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stabilizing lattice oxygen redox in layered sodium transition metal oxide through spin singlet state

Abstract Reversible lattice oxygen redox reactions offer the potential to enhance energy density and lower battery cathode costs. However, their widespread adoption faces obstacles like substantial voltage hysteresis and poor stability. The current research addresses these challenges by achieving a non-hysteresis, long-term stable oxygen redox reaction in the P3-type Na 2/3 Cu 1/3 Mn 2/3 O 2 . Here we show this is accomplished by forming spin singlet states during charge and discharge. Detailed analysis, including in-situ X-ray diffraction, shows highly reversible structural changes during cycling. In addition, local CuO 6 Jahn-Teller distortions persist throughout, with dynamic Cu-O bond length variations. In-situ hard X-ray absorption and ex-situ soft X-ray absorption study, along with density function theory calculations, reveal two distinct charge compensation mechanisms at approximately 3.66 V and 3.99 V plateaus. Notably, we observe a Zhang-Rice-like singlet state during 3.99 V charging, offering an alternative charge compensation mechanism to stabilize the active oxygen redox reaction.

25 ENERGY STORAGE↗

Strong electron-phonon coupling driven pseudogap modulation and density-wave fluctuations in a correlated polar metal

Abstract There is tremendous interest in employing collective excitations of the lattice, spin, charge, and orbitals to tune strongly correlated electronic phenomena. We report such an effect in a ruthenate, Ca 3 Ru 2 O 7 , where two phonons with strong electron-phonon coupling modulate the electronic pseudogap as well as mediate charge and spin density wave fluctuations. Combining temperature-dependent Raman spectroscopy with density functional theory reveals two phonons, B 2 P and B 2 M , that are strongly coupled to electrons and whose scattering intensities respectively dominate in the pseudogap versus the metallic phases. The B 2 P squeezes the octahedra along the out of plane c -axis, while the B 2 M elongates it, thus modulating the Ru 4d orbital splitting and the bandwidth of the in-plane electron hopping; Thus, B 2 P opens the pseudogap, while B 2 M closes it. Moreover, the B 2 phonons mediate incoherent charge and spin density wave fluctuations, as evidenced by changes in the background electronic Raman scattering that exhibit unique symmetry signatures. The polar order breaks inversion symmetry, enabling infrared activity of these phonons, paving the way for coherent light-driven control of electronic transport.

36 MATERIALS SCIENCE↗

Infrared-active phonon modes in single-crystal thorium dioxide and uranium dioxide

The infrared-active phonon modes, in single-crystal samples of thorium dioxide (ThO 2 ) and uranium dioxide (UO 2 ), were investigated using spectroscopic ellipsometry and compared with density functional theory. Both ThO 2 and UO 2 are found to have one infrared-active phonon mode pair [consisting of one transverse optic (TO) and one associated longitudinal optic (LO) mode], which is responsible for the dominant features in the ellipsometric data. Furthermore, at room temperature, our results for the mode pair’s resonant frequencies and broadening parameters are comparable with previous reflectance spectroscopy characterizations and density functional theory predictions. For ThO 2 , our ellipsometry and density function theory results both show that the LO mode broadening parameter is larger than the TO mode broadening. This signifies mode anharmonicity, which can be attributed to the intrinsic phonon–phonon interaction. In addition to the main mode pair, a broad low-amplitude impurity-like vibrational mode pair is detected within the reststrahlen band for both ThO 2 and UO 2 . Elevated temperature measurements were performed for ThO 2 in order to study the mechanisms by which the phonon parameters evolve with increased heat. The observed change in the TO resonant frequency is in excellent agreement with previous density functional calculations, which only consider volume expansion of the crystal lattice. This suggests that the temperature-dependent change in the TO frequency is primarily due to volume expansion. The change in the main mode pair’s broadening parameters is nearly linear within the temperature range of this study, which indicates the intrinsic anharmonic scattering (via cubic anharmonicities) as the main decay mechanism.

36 MATERIALS SCIENCE↗

Structural and electronic changes in L⁢i 2 ⁢Ru⁢O 3 induced by lithium intercalation

Despite extensive research on oxide battery cathodes that transcend classical cationic redox activity, the detailed interplay between structural transformations and electronic redox processes remains insufficiently understood. We report a detailed study of the sequential structural and electronic changes in Li 2 RuO 3 upon lithium intercalation, characterized by powder x-ray and neutron diffraction alongside Ru and O K-edge x-ray absorption spectroscopy (XAS), and guided by operando synchrotron x-ray diffraction. During delithiation, Li 2 RuO 3 evolves from a well-defined monoclinic state to a complex trigonal phase via multiple intermediate structures, marked by significant changes in Ru-O bond distances that closely track the transition from a classical cationic redox to an unconventional process centered at oxygen states. Armed with high-quality atomic structural descriptions, computational models of the O K-edge XAS closely reproduce the experimentally observed spectral shifts. Lastly, we relate observations of electrochemical hysteresis with concurrent changes in the pathways of structural and electronic transitions. In conclusion, our results not only clarify the mechanisms underpinning voltage hysteresis in a model for lattice oxygen redox but also underscore the importance of structural fidelity in modeling redox behavior when this type of complex reactivity is present.

Li, Haifeng [Univ. of Illinois, Chicago, IL (Unite↗

CO Oxidation Mechanisms on CoO x -Pt Thin Films

The reaction of CO and O 2 with submonolayer and multilayer CoO x films on Pt(111), to produce CO 2 , was investigated at room temperature in the mTorr pressure regime. Here, using operando ambient pressure X-ray photoelectron spectroscopy and high pressure scanning tunneling microscopy, as well as density functional theory calculations, we found that the presence of oxygen vacancies in partially oxidized CoO x films significantly enhances the CO oxidation activity to form CO 2 upon exposure to mTorr pressures of CO at room temperature. In contrast, CoO films without O-vacancies are much less active for CO 2 formation at RT, and CO only adsorbed in the form of carbonate species that are stable up to 260 °C. On submonolayer CoO x islands, the carbonates form preferentially at island edges, deactivating the edge sites for CO 2 formation, even while the reaction proceeds inside the islands. These results provide a detailed understanding of CO oxidation pathways on systems where noble metals such as Pt interact with reducible oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Connecting mechanical properties to hydrogen defects in PAN-based carbon fibers

Atomic-level defects dictate the mechanical properties of carbon fibers and strong correlations have been established between the crystallite sizes and mechanical properties. We recently demonstrated similar correlations with hydrogen content, but reliably quantifying the hydrogen content is not possible using only inelastic neutron scattering experiments. Here, we present prompt-gamma activation analysis (PGAA) experiments collected on 20 commercially available carbon fibers to quantify the hydrogen content of carbon fibers and find correlations between fiber modulus and hydrogen content. We then evaluate the role of hydrogen defect type and connect the PGAA results to both newly acquired and recently reported inelastic neutron scattering experiments. In conclusion, we find that intercalated hydrogen defects are preferentially removed at carbonization temperatures required for high-modulus fibers, potentially giving rise to voids within the carbon fibers that undermine their tensile strength.

36 MATERIALS SCIENCE↗

Visualizing Anisotropic Oxygen Diffusion in Ceria under Activated Conditions

Oxygen reactivity plays a key role in the performance of ceria-based catalysts. Aberration-corrected transmission electron microscopy and molecular dynamics simulations were used to study the oxygen atom diffusion in ceria under activated conditions. Reactive oxygen atom and its real-time diffusion were visualized. Additionally, the interplay between cerium and oxygen atoms originating from a Coulomb interaction was revealed by the out-of-plane buckling of cerium atoms associated with oxygen transport. Anisotropic oxygen atom diffusion that depends on crystal orientations was discovered, demonstrating a preferential [001] crystallographic diffusion pathway. These findings reveal prospects for applications of anisotropic orientation-relevant fluorite-structured oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mo Atom Rearrangement Drives Layer-Dependent Reactivity in Two-Dimensional MoS 2

Two-dimensional (2D) materials offer a valuable platform for manipulating and studying chemical reactions at the atomic level, owing to the ease of controlling their microscopic structure at the nanometer scale. While extensive research has been conducted on the structure-dependent chemical activity of 2D materials, the influence of structural transformation during the reaction has remained largely unexplored. In this work, we report the layer-dependent chemical reactivity of MoS 2 during a nitridation atomic substitution reaction and attribute it to the rearrangement of Mo atoms. Our results show that the chemical reactivity of MoS 2 decreases as the number of layers is reduced in the few-layer regime. In particular, monolayer MoS 2 exhibits significantly lower reactivity compared with its few-layer and multilayer counterparts. Atomic-resolution transmission electron microscopy (TEM) reveals that MoN nanonetworks form as reaction products from monolayer and bilayer MoS 2 , with the continuity of the MoN crystals increasing with layer number, consistent with the local conductivity mapping data. The layer-dependent reactivity is attributed to the relative stability of the hypothetically formed MoN phase, which retains the number of Mo atomic layers present in the precursor. Specifically, the low chemical reactivity of monolayer MoS 2 is attributed to the high energy cost associated with Mo atom diffusion and migration necessary to form multilayer Mo lattices in the thermodynamically stable MoN phase. In conclusion, this study underscores the critical role of lattice rearrangement in governing chemical reactivity and highlights the potential of 2D materials as versatile platforms for advancing the understanding of materials chemistry at the atomic scale.

Chemical reactivity↗

Fermi surface reconstruction due to orthorhombic distortion in the Dirac semimetal YbMnSb 2

A Dirac semimetal with magnetic atoms as constituents delivers an interesting platform to investigate the interplay of Fermi surface (FS) topology, electron correlation, and magnetism. One such family of semimetals is YbMn⁢ 𝑃⁢𝑛 2 (𝑃⁢𝑛 = Sb,Bi), which is being actively studied due to the intertwined spin and charge degrees of freedom. Here, in this study, we investigate the relationship between the magnetic/crystal structures and FS topology of YbMnSb 2 using single crystal x-ray diffraction, neutron scattering, magnetic susceptibility, magnetotransport measurements, and complimentary density functional theory (DFT) calculations. Contrary to previous reports, the x-ray and neutron diffraction reveal that YbMnSb 2 crystallizes in an orthorhombic 𝑃⁢𝑛⁢𝑚⁢𝑎 structure with a notable antiphase displacement of the magnetic Mn ions that increases in magnitude upon cooling. As a result of this orthorhombicity, first-principles DFT calculation reveals a reduced Brillouin zone and more anisotropic FS of YbMnSb 2 compared to YbMnBi 2 . Moreover, the hole-type carrier density drops by two orders of magnitude as YbMnSb 2 orders antiferromagnetically, indicating band folding in a magnetic ordered state. In addition, the Landau level fan diagram yields a nontrivial nature of the Shubnikov–de Haas quantum oscillation frequency arising from the Dirac-like Fermi pocket. These results imply that YbMnSb 2 is an ideal platform to explore the interplay of subtle lattice distortion, magnetic order, and topological transport arising from relativistic quasiparticles.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Computationally designed coiled coil ‘bundlemers’ as model colloidal nanoparticles for solution assembly and materials design (Final Report)

As a collaborative team at the University of Delaware and the University of Pennsylvania, Kloxin, Pochan and Saven designed new biomimetic nanomaterials de novo, leveraging a variety of complementary areas of expertise: computational design of biopolymers (Saven at the University of Pennsylvania), and synthesis and characterization (Kloxin and Pochan at the University of Delaware). Overall activities included: sequence-specific peptide synthesis; covalent crosslinking; noncovalent assembly; site-specific functionalization; and nanostructural characterization using electron microscopy and solution-phase (x-ray and neutron) scattering. Using natural and non-natural amino acids, the team created modular, functional peptide building blocks for elaboration of new nanostructured materials. Ultimately, the development of robust peptide-based, building blocks provides tools for researchers to readily produce complex nanomaterial structures in a wide range of applications. The project had three, interconnecting goals in an effort to provide the broader scientific community with a new peptide-based paradigm for materials design and characterization. First, we further developed the coiled-coil bundle-based toolbox (otherwise known as the ‘bundlemer’ toolbox) via computational design with experimental bundle assembly verification. Second, we developed new uses of covalent interactions, in addition to desired physical (noncovalent) interactions, to assemble bundlemers into 1-D polymer chains with targeted chain rigidity, length, and dispersity. Thirds, we used the above designs to experimentally realize (physical or covalent) polymers to target the creation of liquid crystals or to realize interparticle assembly into nanoporous lattices. The close integration of the three groups was instrumental in success of the biomolecular materials design, formation, and understanding for future designs.

36 MATERIALS SCIENCE↗

Topological magnons and topological electronic properties in metallic Kagome magnets

The primary goal of this project is to study metallic Kagome magnets that potentially host topological electronic properties and topological magnetic excitations, aiming to understand the effect of lattice geometry on topological character of magnons and electronic bands and to study the interplay between magnetism and topological electronic properties. Through this DOE-funded research program, we have unraveled novel electronic and thermoelectric properties of RMn 6 Sn 6 (R = Y, Tb, and Er) and Fe 3 Ge Kagome magnets, including anomalous Hall effect and anomalous Nernst effect, which are associated with the Berry curvature contribution from the massive Dirac gaps in the 3D momentum space. In addition, we have also revealed topological Hall effect and topological Nernst effect, and we ascribed these phenomena to the Berry curvature associated with the magnetic field-induced non-zero scalar spin chirality. These features highlight the synergic effects of the Berry phases in both momentum space and real space of Kagome magnets, which render them excellent candidates for room-temperature electronic and thermoelectric applications based on transverse transport. In addition, through this program we have also study novel thermal transport properties of quantum materials by probing the thermal Hall effect, which can provide crucial insights into nontrivial topological character and chirality of quasiparticles like magnons and magnon-polarons. This report provides an overview of some project activities related to these accomplishments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electronic Structure of Excitons in Hematite Fe 2 O 3

We present a computational study of the electronic structure of excitons in hematite Fe 2 O 3 using density functional theory (DFT) and time-dependent DFT theory. Excitons resulting from solar light absorption are precursors to photogenerated charge carriers, which are the active species in solar-to-fuel redox conversions. Upon vertical excitation, the lowest energy exciton is found to have a multideterminantal wave function, describing an electron excited from O 2p states to Fe 3d states of the nearest basal plane, possibly supporting a recent XUV-derived exciton structure with a radius of a single Fe–O bond. Subsequently, the exciton self-traps into stable electron–hole pair structures whose wave functions are well-approximated by single excitations conveniently labeled “HOMO–LUMO”. Self-trapping yields electron–hole pair structures whereby the electron state (electron polaron-like) is separated from the hole state (hole polaron-like) by 3, 5, 7, 9, ... basal planes in structures referred to as Exc-3, Exc-5, Exc-7, Exc-9, ... The natural transition orbitals (electron–hole states) exhibit a strong “localized” character. The hole state is best described as a (FeO 6 ) + octahedral moiety carrying ~0.65 h + charge, and overall ~70% of the hole is assigned to O 2p atomic states, mostly on the four (4) equatorial O atoms of the moiety. The electron state is best described as a (FeFe) – moiety carrying ~0.80 e – charge in Fe 3d atomic states. The lattice distortions around the hole site exhibit Fe–O bond shortening due to the removal of electron density from an orbital state with O–Fe–O antibonding character. The electron site shows Fe–Fe distance shortening due to excess electron density added to an orbital state with in-phase Fe–Fe interactions. Furthermore, these excitonic structures with increasing electron–hole separation can be viewed as the onset of exciton separation into isolated electrons and hole polarons.

36 MATERIALS SCIENCE↗

Understanding the Re-entrant Phase Transition in a Non-magnetic Scheelite

We report the stereochemical activity of lone pair electrons plays a central role in determining the structural and electronic properties of both chemically simple materials such as H 2 O, as well as more complex condensed phases such as photocatalysts or thermoelectrics. TlReO 4 is a rare example of a non-magnetic material exhibiting a re-entrant phase transition and emphanitic behavior in the long-range structure. Here, we describe the role of the Tl + 6s 2 lone pair electrons in these unusual phase transitions and illustrate its tunability by chemical doping, which has broad implications for functional materials containing lone pair bearing cations. First-principles density functional calculations clearly show the contribution of the Tl + 6s 2 in the valence band region. Local structure analysis, via neutron total scattering, revealed that changes in the long-range structure of TlReO 4 occur due to changes in the correlation length of the Tl + lone pairs. This has a significant effect on the anion interactions, with long-range ordered lone pairs creating a more densely packed structure. This resulted in a trade-off between anionic repulsions and lone pair correlations that lead to symmetry lowering upon heating in the long-range structure, whereby lattice expansion was necessary for the Tl + lone pairs to become highly correlated. Similarly, introducing lattice expansion through chemical pressure allowed long-range lone pair correlations to occur over a wider temperature range, demonstrating a method for tuning the energy landscape of lone pair containing functional materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stability of Pt Skin Intermetallic Core Catalysts and Adsorption Properties for the Oxygen Reduction Reaction

Density functional theory calculations were used to determine the stability of metal slabs consisting of a Pt surface monolayer and intermetallic supporting layers made from combinations of six transition metal elements (Pt, Fe, Co, Ni, Cu, and Ag), as a model system for Pt skin intermetallic core nanoparticle catalysts. The stability of the slabs is largely determined by strain at the interface of the Pt skin and the subsurface intermetallic, which was described by a lattice matching parameter (r). The surface charge on the Pt skin was found to be correlated with the average electronegativity (EN) of the intermetallic core, so this average EN was used as a descriptor for how the electronic coupling (or ligand effect) affects adsorption energies. A total of 46 slabs were investigated in terms of their stability, from which 10 stable slabs were selected for further studies of adsorbate binding (OOH*, O*, and OH*) that are intermediates in the oxygen reduction reaction (ORR). The correlation between all three adsorption energies and descriptors r and EN was found. Using a linear fit between our descriptors and the calculated adsorption energies, the overpotential for the ORR was obtained as a function of r and EN, from which a volcano plot was produced. The volcano peak was found at r = 0.96 or at EN = 2.025. Interestingly, neither r nor EN was a sufficient single reactivity descriptor as the data points were well off the general trend in both linear fits; this implies that both the strain effect and the ligand effect influence the adsorption energies, although they are partly correlated. The (r, EN) target peak parameters were used to screen over 241 intermetallic combinations of transition metal elements as active ORR activity. In conclusion, this analysis identified 11 intermetallic compounds which can support a Pt skin to have a high predicted ORR activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

An Integrated Multiscale Experimental-Numerical Analysis on Reconsolidation of Salt-Clay Mixture for Disposal of Heat-Generating Waste (Final NEUP Technical Report)

The overall purpose of this research is to improve understanding of THMC coupling effect on the reconsolidation of granular (or crushed) salt-clay mixture used for seal systems of shafts and drifts in salt repositories. This proposed work is partially motivated by the recent work on the Waste Isolation Pilot Plant (WIPP) that shows the promising sealing capability of clay-salt mixture compared to crushed salt. In particular, primary emphasis is to develop a fully integrated multiscale experiment-numerical study to determine and explain what leads to the superior sealing ability of the clay-salt mixture. These research activities are designed to seek further understanding of (1) why clay additives may enhance the fluid trapping and (2) whether this flow barrier effect may prevail under different combinations of temperature, confining pressure, deviatoric stress and other foreseeable environmental factors. If successful, this enhanced flow trapping ability of the seal provides significant improvement to the seal and repository performance and therefore make the repository safer in the long-term. The experiment component includes microstructural investigation and macroscopic tests on a reconsolidated salt-clay mixture. In the microstructural study, the goal is to (1) characterize microscopic distributions of distinct phases (e.g., clay, salt crystal boundaries, trapped brine, and pore) to examine the connectivity of the pore network inside the salt-clay mixture with different amounts of clay additive and moisture content and (2) analyze multiscale imaging data to reconstruct the polycrystalline microstructures for numerical simulations. Meanwhile, macroscopic tests are performed to analyze how clay alters the failure/creep mechanisms in the salt-clay mixture. Microscopic and macroscopic experimental observations will both be used to calibrate and validate a multiscale model that explicitly simulates the capillary and multiphase flow in the connected pores and the deformation due to the presence of intra-crystalline brine at the pore scale via a new polyhedral discrete element–lattice Boltzmann method (DEM-LBM) coupling model. The pore-scale simulations are homogenized via an upscaling procedure that converts pore-scale information (e.g. force exerted on grain boundary, sliding, pressure-solution) to continuum measures (e.g. Cauchy stress, Darcy’s flow) at each integration point in the macroscopic multiphase TMHC model. This multiscale scheme will allow coupling be- tween high-fidelity simulations of brine-salt-clay interaction and the macroscopic TMHC model. The multiscale model helps the understanding of how the trapped brine inclusion affects the pressure-solution mechanism with the presence of clay and moisture. This work brings new insight into the sealing capacity of salt-clay mixture under elevated temperature over a long period of time - a key to evaluating the potential of salt-clay mixture usage for salt repositories.

42 ENGINEERING↗