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Title: Mitigating mechanical failure of crystalline silicon electrodes for lithium batteries by morphological design [Morphological design of silicon electrode with anisotropic interface reaction rate for lithium ion batteries]

Although crystalline silicon (c-Si) anodes promise very high energy densities in Li-ion batteries, their practical use is complicated by amorphization, large volume expansion and severe plastic deformation upon lithium insertion. Recent experiments have revealed the existence of a sharp interface between crystalline Si (c-Si) and the amorphous LixSi alloy during lithiation, which propagates with a velocity that is orientation dependent; the resulting anisotropic swelling generates substantial strain concentrations that initiate cracks even in nanostructured Si. Here we describe a novel strategy to mitigate lithiation-induced fracture by using pristine c-Si structures with engineered anisometric morphologies that are deliberately designed to counteract the anisotropy in the crystalline/amorphous interface velocity. This produces a much more uniform volume expansion, significantly reducing strain concentration. Based on a new, validated methodology that improves previous models of anisotropic swelling of c-Si, we propose optimal morphological designs for c-Si pillars and particles. The advantages of the new morphologies are clearly demonstrated by mesoscale simulations and verified by experiments on engineered c-Si micropillars. The results of this study illustrate that morphological design is effective in improving the fracture resistance of micron-sized Si electrodes, which will facilitate their practical application in next-generation Li-ion batteries. In conclusion, the model and designmore » approach present in this paper also have general implications for the study and mitigation of mechanical failure of electrode materials that undergo large anisotropic volume change upon ion insertion and extraction.« less
 [1] ;  [2] ;  [2] ;  [3] ;  [2] ;  [4] ;  [5]
  1. Arizona State Univ., Tempe, AZ (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  4. Rice Univ., Houston, TX (United States)
  5. Arizona State Univ., Mesa, AZ (United States)
Publication Date:
OSTI Identifier:
Report Number(s):
Journal ID: ISSN 1463-9076; PPCPFQ
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 17; Journal Issue: 27; Journal ID: ISSN 1463-9076
Royal Society of Chemistry
Research Org:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States