arXiv subjects

Giovanna Bucci

Publications and source records attributed to Giovanna Bucci.

8 recordsLinked to original sources

arXiv2026

A Poromechanics-Based Framework for Fully Coupled Reactive Transport and Geomechanics in Porous Rocks

Mineral precipitation and dissolution in rocks alter pore structure, stress, and hydraulic properties, producing tightly coupled chemo-hydro-mechanical processes that are central to subsurface systems. Yet, existing continuum-scale simulators lack a generalizable, mathematically tractable, and physically grounded chemo-mechanics formulation for modeling these coupled processes. To address this gap, this work presents a poromechanics-based framework for chemo-mechanics coupling and integrates it into coupled reactive transport and geomechanics simulations. Building upon classical poromechanics theory, the framework provides distinct descriptions for the stress states of the host rock, pore fluid, and pore minerals, enabling a rigorous and flexible treatment of their individual behavior and mechanical interactions during precipitation and dissolution. As demonstrated by numerical examples, the poromechanics-based method captures the expected mechanical response by translating pore-scale mineral growth into mineralization pressure. By accounting for mineral compressibility, the method also supports more physically realistic representations of deformation and induced stress. Comparisons with the eigenstrain method further highlight the unique capability of the poromechanics-based approach to model effective stress evolution and fracture development without explicitly representing pore geometry or other microstructural features. Overall, this framework offers a versatile, physics-based predictive approach to modeling coupled chemo-mechanical processes in reactive porous rocks and supports future reservoir-scale analyses of engineered subsurface systems.

physics.geo-ph↗

arXiv2026

Scalable Preconditioners for the Pseudo-4D DFN Lithium-ion Battery Model

The pseudo-4D Doyle-Fuller-Newman (DFN) model enables predictive simulation of lithium-ion batteries with three-dimensional electrode architectures and particle-scale diffusion, extending the standard pseudo-2D (P2D) formulation to fully resolve cell geometry. This leads to large, nonlinear systems with strong coupling across multiple physical scales, posing significant challenges for scalable numerical solution. We introduce block-structured preconditioning strategies that exploit the mathematical properties of the coupled system, employing multigrid techniques for electrode-level operators and localized solvers for particle-scale diffusion. Comprehensive scalability studies are performed across a range of geometries, including homogeneous and heterogeneous cubic cells, flattened jelly-roll configurations, and triply periodic minimal surface electrodes, to assess solver robustness and parallel scalability. The proposed methods consistently deliver efficient convergence and enable the solution of battery models with hundreds of millions of degrees of freedom on large-scale parallel hardware.

math.NA↗

arXiv2024

Topology Optimization for the Full-Cell Design of Porous Electrodes in Electrochemical Energy Storage Devices

In this paper, we introduce a density-based topology optimization framework to design porous electrodes for maximum energy storage. We simulate the full cell with a model that incorporates electronic potential, ionic potential, and electrolyte concentration. The system consists of three materials, namely pure liquid electrolyte and the porous solids of the anode and cathode, for which we determine the optimal placement. We use separate electronic potentials to model each electrode, which allows interdigitated designs. As a result, a penalization is required to ensure that the anode and cathode do not touch, i.e., causing a short circuit. We compare multiple 2D designs generated for different fixed conditions, e.g. material properties. A 3D design with complex channel and interlocked structure is also created. All optimized designs are far superior to the traditional monolithic electrode design with respect to energy storage metrics. We observe up to a 750% increase in energy storage for cases with slow effective ionic diffusion within the porous electrode.

physics.app-ph↗

arXiv2024

Shape matters: Understanding the effect of electrode geometry on cell resistance and chemo-mechanical stress

Rechargeable batteries that incorporate shaped three-dimensional electrodes have been shown to have increased power and energy densities for a given footprint area when compared to a conventional geometry, i.e., a planar cathode and anode that sandwich an electrolyte. Electrodes can be shaped to enable a higher loading of active material, while keeping the ion transport distance small, however, the relationship between electrical and mechanical performance remains poorly understood. A variety of electrode shapes have been explored, where the electrodes are individually shaped or intertwined with one another. Advances in manufacturing and shape and topology optimization have made such designs a reality. In this paper, we explore sinusoidal half cells and interdigitated full cells. First, we use a simple electrostatics model to understand the cell resistance as a function of shape. We focus on low-temperature conditions, where the electrolyte conductivity decreases and the governing dimensionless parameters change. Next, we use a chemo-mechanics model to examine the stress concentrations that arise due to intercalation-driven volume expansion. We show that shaped electrodes provide a significant reduction in resistance, however, they result in unfavorable stress concentrations. Overall, we find that the fully interdigitated electrodes may provide the best balance with respect to this trade-off.

physics.chem-ph↗

arXiv2022

Modeling of porous lithium metal electrodes: turning the Li-dendrite problem around

The properties of rechargeable lithium-ion batteries are determined by the electrochemical and kinetic properties of their constituent materials as well as by their underlying microstructure. Microstructural design can be leveraged to achieve a leap in performance and durability. Here we investigate a porous electrode structure, as a strategy to increase the surface area, and provide structural stability for Li-metal anodes. The porous architecture consists of a mixed electron/ion conductor that function as a scaffold for lithium metal deposition. A new finite element model was developed to simulate the large topological changes associated with Li plating/stripping. This model is used to predict the current density distribution as a function of material and structural properties. A dimensionless quantity that combines Li-ion conductivity, surface impedance and average pore size is shown to be a good indicator to predict the peak current density. Preventing current localization at the separator reduces the risk of cell shorting. The analyses show that the peak current scales as $(hG)^{1/2}$, where $h$ is the ratio between surface and bulk conductivity and $G$ is the average pore size. Stability analyses suggest that the growth is morphologically stable, and that confining Li-plating into pores can enable high-energy density solid-state batteries. In addition to optimizing porous electrodes design, this finite element method can be extended to studying other Li-battery structures.

cond-mat.mtrl-sci↗

arXiv2017

Modeling of internal mechanical failure of all-solid-state batteries during electrochemical cycling, and implications for battery design

This is the first quantitative analysis of mechanical reliability of all-solid state batteries. Mechanical degradation of the solid electrolyte (SE) is caused by intercalation-induced expansion of the electrode particles, within the constrain of a dense microstructure. A coupled electro-chemo-mechanical model was implemented to quantify the material properties that cause a SE to fracture. The treatment of microstructural details is essential to the understanding of stress-localization phenomena and fracture. A cohesive zone model is employed to simulate the evolution of damage. In the numerical tests, fracture is prevented only if electrode-particle's expansion is lower than 7.5% and the solid-electrolyte's fracture energy higher than $G_c = 4$ J m$^{-2}$. Perhaps counter-intuitively, the analyses show that compliant solid electrolytes (with Young's modulus in the order of E$_{SE} = 15$ GPa) are more prone to micro-cracking. This result, captured by our non-linear kinematics model, contradicts the speculations that sulfide SEs are more suitable for the design of bulk-type batteries than oxide SEs. Mechanical degradation is linked to the battery power-density. Fracture in solid Li-ion conductors represents a barrier for Li transport, and accelerates the decay of rate performance.

cond-mat.mtrl-sci↗

arXiv2013

Measurement and modeling of the mechanical and electrochemical response of amorphous Si thin film electrodes during cyclic lithiation

A combination of experimental measurements and numerical simulations are used to characterize the mechanical and electrochemical response of thin film amorphous Si electrodes during cyclic lithiation. Parameters extracted from the experiment include the variation of elastic modulus and the flow stress as functions of Li concentration; the strain rate sensitivity; the diffusion coefficient for Li transport in the electrode; the free energy of mixing as a function of Li concentration in the electrode; the exchange current density for the Lithium insertion reaction; as well as reaction rates and diffusion coefficients characterizing the rate of formation of solid-electrolyte interphase layer at the electrode surface. Model predictions are compared with experimental measurements; and the implications for practical Si based electrodes are discussed.

cond-mat.mtrl-sci↗

arXiv2013

On plastic deformation and fracture in Si films during electrochemical lithiation/delithiation cycling

An in situ study of deformation, fracture, and fatigue behavior of silicon as a lithium-ion battery electrode material is presented. Thin films (100-200 nm) of silicon are cycled in a half-cell configuration with lithium metal foil as counter/reference electrode, with 1M lithium hexafluorophosphate in ethylene carbonate, diethylene carbonate, dimethyl carbonate solution (1:1:1, wt.%) as electrolyte. Stress evolution in the Si thin-film electrodes during electrochemical lithiation and delithiation is measured by monitoring the substrate curvature using the multi-beam optical sensing method. The stress measurements have been corrected for contributions from residual stress arising from sputter-deposition. An indirect method for estimating the potential errors due to formation of the solid-electrolyte-interphase layer and surface charge on the stress measurements was presented. The films undergo extensive inelastic deformation during lithiation and delithiation. The peak compressive stress during lithiation was 1.48 GPa. The stress data along with the electron microscopy observations are used to estimate an upper bound fracture resistance of lithiated Si, which is approximately 9-11 J/m^2. Fracture initiation and crack density evolution as a function of cycle number is also reported.

cond-mat.mtrl-sci↗