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• W3150455925 abstract "Li-ion batteries is asystem that dynamically couples electrochemistry and mechanics. The electrochemicalprocesses occurring during battery operation induces a wealth of elementalmechanics such as deformation, plasticity, and fracture. Likewise, mechanicsinfluences the electrochemical processes via modulating the thermodynamics ofLi reactions and kinetics of ionic transport. These complex interrelatedphenomena are far from being well understood and need to be further explored.This thesis studies the couplings between the mechanical phenomena andelectrochemical processes in Li-ion batteries using integrated theories andexperiments. A continuum model couplingthe kinetics of Li diffusion and kinematics of large elasto-plastic deformationis established to investigate the coupling between Li transport and stressevolution in electrodes of Li-ion batteries. Co-evolutions of Li distribution,stress field and deformation in the electrodes with multiple components areobtained. It is found that the Li profile and stress state in a compositeelectrode are significantly different from that ina free-standing configuration, mainly due to the regulation from the mechanicalinteractions between different components. Chemomechanical behaviors of theheterogeneous electrodes in real batteries are further explored. Three-dimensionalreconstructed models are employed to investigate the mechanical interactions ofthe constituents and their influence on the accessible capacity of batteries. Structural disintegration of thestate-of-art cathode materials LiNixMnyCozO2(x+y+z=1, NMC) during electrochemical cycling is experimentally revealed. Microstructuralevolution of different marked regimes in electrodes are tracked before and afterlithiation cycles. It is found that the decohesion of primary particlesconstitutes the major mechanical degradation in the NMC materials. Electrochemicalimpedance spectroscopy (EIS) measurement confirms that the mechanicaldisintegration of NMC secondary particle causes the electrochemical degradationof the battery. To reveal the reasons for particle disintegration, the dynamicevolution of mechanical properties of NMC during electrochemical cycling isexplored by using instrumented nanoindentation. It is found that the elasticmodulus, hardness, and interfacial fracture strength of NMC secondary particlesignificantly depend on the lithiation state and degrade as the electrochemicalcycles proceed, which may cause the damage accumulation during battery cycling.Corrosive fracture of electrodes inLi-ion batteries is investigated. Li reaction causes embrittlement of the hostmaterial and typically results in a decrease of fracture toughness. Thedynamics of crack growth depends on the chemomechanical load, kinetics of Litransport, and the Li embrittlement effect. A theory of coupled diffusion,large deformation, and crack growth is implemented into finite element programand the corrosive fracture of electrodes under concurrent mechanical andchemical load is simulated. The competition between energy release rate andfracture resistance as crack grows during both Li insertion and extraction isexamined in detail, and it is found that the corrosive fracture behaviors ofthe electrodes rely on the chemomechanical load and the supply of Li to thecrack tip. The theory is further applied to model corrosive behavior ofintergranular cracks in NMC upon Li cycles. The evolving interfacial strengthat different states of charge and different cycle numbers measured by in-situnanoindentation is implemented in the numerical simulation." @default.
• W3150455925 created "2021-04-13" @default.
• W3150455925 creator A5075914865 @default.
• W3150455925 date "2019-01-17" @default.
• W3150455925 modified "2023-09-24" @default.
• W3150455925 title "Theories and Experiments on the Electro-Chemo-Mechanics of Battery Materials" @default.
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