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1. Modeling Multiphase Flow Within and Around Deformable Porous Materials: A Darcy‐Brinkman‐Biot Approach

   https://doi.org/10.1029/2020WR028734  

   Carrillo, Francisco J. ; Bourg, Ian C. ( February 2021 , Water Resources Research)

   We present a new computational fluid dynamics approach for simulating two‐phase flow in hybrid systems containing solid‐free regions and deformable porous matrices. Our approach is based on the derivation of a unique set of volume‐averaged partial differential equations that asymptotically approach the Navier‐Stokes Volume‐of‐Fluid equations in solid‐free regions and multiphase Biot Theory in porous regions. The resulting equations extend our recently developed Darcy‐Brinkman‐Biot framework to multiphase flow. Through careful consideration of interfacial dynamics (relative permeability and capillary effects) and extensive benchmarking, we show that the resulting model accurately captures the strong two‐way coupling that is often exhibited between multiple fluids and deformable porous media. Thus, it can be used to represent flow‐induced material deformation (swelling, compression) and failure (cracking, fracturing). The model's open‐source numerical implementation,hybridBiotInterFoam, effectively marks the extension of computational fluid mechanics into modeling multiscale multiphase flow in deformable porous systems. The versatility of the solver is illustrated through applications related to material failure in poroelastic coastal barriers and surface deformation due to fluid injection in poro‐visco‐plastic systems.

    

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2. Chemistry–mechanics–geometry coupling in positive electrode materials: a scale-bridging perspective for mitigating degradation in lithium-ion batteries through materials design

   https://doi.org/10.1039/d2sc04157j  

   Santos, David A. ; Rezaei, Shahed ; Zhang, Delin ; Luo, Yuting ; Lin, Binbin ; Balakrishna, Ananya R. ; Xu, Bai-Xiang ; Banerjee, Sarbajit ( January 2023 , Chemical Science)

   Despite their rapid emergence as the dominant paradigm for electrochemical energy storage, the full promise of lithium-ion batteries is yet to be fully realized, partly because of challenges in adequately resolving common degradation mechanisms. Positive electrodes of Li-ion batteries store ions in interstitial sites based on redox reactions throughout their interior volume. However, variations in the local concentration of inserted Li-ions and inhomogeneous intercalation-induced structural transformations beget substantial stress. Such stress can accumulate and ultimately engender substantial delamination and transgranular/intergranular fracture in typically brittle oxide materials upon continuous electrochemical cycling. This perspective highlights the coupling between electrochemistry, mechanics, and geometry spanning key electrochemical processes: surface reaction, solid-state diffusion, and phase nucleation/transformation in intercalating positive electrodes. In particular, we highlight recent findings on tunable material design parameters that can be used to modulate the kinetics and thermodynamics of intercalation phenomena, spanning the range from atomistic and crystallographic materials design principles (based on alloying, polymorphism, and pre-intercalation) to emergent mesoscale structuring of electrode architectures (through control of crystallite dimensions and geometry, curvature, and external strain). This framework enables intercalation chemistry design principles to be mapped to degradation phenomena based on consideration of mechanics coupling across decades of length scales. Scale-bridging characterization and modeling, along with materials design, holds promise for deciphering mechanistic understanding, modulating multiphysics couplings, and devising actionable strategies to substantially modify intercalation phase diagrams in a manner that unlocks greater useable capacity and enables alleviation of chemo-mechanical degradation mechanisms. 

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3. Continuum approximation of dyking with a theory for poro-viscoelastic–viscoplastic deformation

   https://doi.org/10.1093/gji/ggad173  

   Li, Yuan ; Pusok, Adina E. ; Davis, Timothy ; May, Dave A. ; Katz, Richard F. ( April 2023 , Geophysical Journal International)

   To reach Earth’s surface, magma must ascend from the hot, ductile asthenosphere through cold and brittle rock in the lithosphere. It does so via fluid-filled fractures called dykes. While the continuum mechanics of ductile asthenosphere is well established, there has been little theoretical work on the cold and brittle regime where dyking and faulting occurs. Geodynamic models use plasticity to model fault-like behaviour; plasticity also shows promise for modelling dykes. Here we build on an existing model to develop a poro-viscoelastic–viscoplastic theory for two-phase flow across the lithosphere. Our theory addresses the deficiencies of previous work by incorporating (i) a hyperbolic yield surface, (ii) a plastic potential with control of dilatancy and (iii) a viscous regularization of plastic failure. We use analytical and numerical solutions to investigate the behaviour of this theory. Through idealized models and a comparison to linear elastic fracture mechanics, we demonstrate that this behaviour includes a continuum representation of dyking. Finally, we consider a model scenario reminiscent of continental rifting and demonstrate the consequences of dyke injection into the cold, upper lithosphere: a sharp reduction in the force required to rift.

    

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4. Electrodeposition Stability Landscape for Solid–Solid Interfaces

   https://doi.org/10.1002/advs.202307455  

   Chatterjee, Debanjali ; Naik, Kaustubh G. ; Vishnugopi, Bairav S. ; Mukherjee, Partha P. ( December 2023 , Advanced Science)

   As solid‐state batteries (SSBs) with lithium (Li) metal anodes gain increasing traction as promising next‐generation energy storage systems, a fundamental understanding of coupled electro‐chemo‐mechanical interactions is essential to design stable solid‐solid interfaces. Notably, uneven electrodeposition at the Li metal/solid electrolyte (SE) interface arising from intrinsic electrochemical and mechanical heterogeneities remains a significant challenge. In this work, the thermodynamic origins of mechanics‐coupled reaction kinetics at the Li/SE interface are investigated and its implications on electrodeposition stability are unveiled. It is established that the mechanics‐driven energetic contribution to the free energy landscape of the Li deposition/dissolution redox reaction has a critical influence on the interface stability. The study presents the competing effects of mechanical and electrical overpotential on the reaction distribution, and demarcates the regimes under which stress interactions can be tailored to enable stable electrodeposition. It is revealed that different degrees of mechanics contribution to the forward (dissolution) and backward (deposition) reaction rates result in widely varying stability regimes, and the mechanics‐coupled kinetics scenario exhibited by the Li/SE interface is shown to depend strongly on the thermodynamic and mechanical properties of the SE. This work highlights the importance of discerning the underpinning nature of electro‐chemo‐mechanical coupling toward achieving stable solid/solid interfaces in SSBs.

    

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5. Toward High-Capacity Battery Anode Materials: Chemistry and Mechanics Intertwined

   https://doi.org/10.1021/acs.chemmater.0c02981  

   McDowell, Matthew T. ; Cortes, Francisco Javier ; Thenuwara, Akila C. ; Lewis, John A. ( September 2020 , Chemistry of Materials)

   Lithium metal and lithium-rich alloys are high-capacity anode materials that could boost the energy content of rechargeable batteries. However, their development has been hindered by rapid capacity decay during cycling, which is driven by the substantial structural, morphological, and volumetric transformations that these materials and their interfaces experience during charge and discharge. During these transformations, the interplay between chemical/structural changes and solid mechanics plays a defining role in determining electrochemical degradation. This Perspective discusses how chemistry and mechanics are interrelated in influencing the reaction mechanisms, stability, and performance of both lithium metal anodes and alloy anodes. Battery systems with liquid electrolytes and solid-state electrolytes are considered because of the distinct effects of chemo-mechanics in each system. Building on this knowledge, we present a discussion of emerging ideas to control and mitigate chemo-mechanical degradation in these materials to enable translation to commercial systems, which could lead to the development of high-energy batteries that are urgently needed to power our increasingly electrified world. 

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