Reaction Front Evolution during Electrochemical Lithiation of Crystalline Silicon Nanopillars

Lee, Seok Woo; Berla, Lucas A.; McDowell, Matthew T.; Nix, William D.; Cui, Yi

doi:10.1002/ijch.201200077

Cited by 19 publications

(20 citation statements)

References 32 publications

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“…1 nm, and progressed linearly with time . Lee et al demonstrated an experimental investigation on the anisotropy of the lithiation process. It was revealed that the exposed crystalline cores had flat (110) surfaces at the pillar sidewalls.…”

Section: Methods To Buffer the Challengesmentioning

confidence: 99%

Nanostructured Silicon Anodes for High‐Performance Lithium‐Ion Batteries

Rahman

Song

Bhatt

et al. 2015

Adv Funct Materials

287

167

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Despite the high theoretical capacity of Si anodes, the electrochemical performance of Si anodes is hampered by severe volume changes during lithiation and delithiation, leading to poor cyclability and eventual electrode failure. Nanostructured silicon and its nanocomposite electrodes could overcome this problem holding back the deployment of Si anodes in lithium‐ion batteries (LIBs) by providing facile strain relaxation, short lithium diffusion distances, enhanced mass transport, and effective electrical contact. Here, the recent progress in nanostructured Si‐based anode materials such as nanoparticles, nanotubes, nanowires, porous Si, and their respective composite materials and fabrication processes in the application of LIBs have been reviewed. The ability of nanostructured Si materials in addressing the above mentioned challenges have been highlighted. Future research directions in the field of nanostructured Si anode materials for LIBs are summarized.

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Section: Methods To Buffer the Challengesmentioning

confidence: 99%

Nanostructured Silicon Anodes for High‐Performance Lithium‐Ion Batteries

Rahman

Song

Bhatt

et al. 2015

Adv Funct Materials

287

167

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“…During the initial lithiation process, c-Si and a-Si both undergo two phase lithiation and are transformed to an amorphous Li x Si alloy, separated by a phase boundary, which attributes to the tensile hoop stress state and the appearance of surface cracks of Si electrodes [3,5]. Experimental investigations and theoretical models further show that the different chemical reaction rates in different crystalline directions at the phase boundary cause an anisotropic deformation of Si electrodes [94,95]. This observation further raises the complexity when modeling diffusion induced large plastic deformation and phase field fracture of Si electrodes.…”

Section: Account For Two-phase Lithiationmentioning

confidence: 98%

A variational framework to model diffusion induced large plastic deformation and phase field fracture during initial two-phase lithiation of silicon electrodes

Zhang

Krischok

Linder

2016

Computer Methods in Applied Mechanics and Engineering

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Silicon (Si) is considered as a promising next-generation anode material for lithium-ion batteries. However, the large volume change during (de)lithiation processes causes fracture of Si electrodes, thereby limiting Si's practical application in lithium-ion batteries. In this work, we formulate a variational-based fully chemo-mechanical coupled computational framework to study diffusion induced large plastic deformation and phase field fracture in Si electrodes. Into this framework we incorporate a recently developed reaction-controlled diffusion model to predict two-phase lithiation for amorphous Si (a-Si) and crystalline Si (c-Si) as well as diffusion induced anisotropic deformation for c-Si. The variational formulation suggests to consider the deformation field, chemical potential, and the damage field as primary unknowns. The concentration field is considered as a local variable and is recovered from the chemical potential on the element level. We carry out several numerical simulations to show the performance of our computational model and point out the significance of accurately accounting for the presence of the reaction front when modeling diffusion induced fracture problems for both a-Si and c-Si electrodes. In addition, we investigate how the fracture energy release rate, diffusion coefficient, electrode geometry, and geometrical constraints affect the fracture behavior of Si electrodes.

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“…Especially, silicon has been extensively studied due to its highest specific capacity among alloy anodes and its relative abundance [8][9][10][11][12] . Contradicting the former thought that Si lithiates via isotropic lithium (Li) reaction and diffusion, we recently showed that Si undergoes anisotropic volume expansion, with expansion most significant along <110> directions 13,14 .…”

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confidence: 99%