Journal
NANO LETTERS
Volume 13, Issue 9, Pages 4511-4516Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nl402429a
Keywords
Li-Si alloys; electrochemical solid-state amorphization; ab initio molecular dynamics simulations; in situ TEM; electron rich
Categories
Funding
- DOE's Office of Biological and Environmental Research
- DOE [DE-AC05-76RLO1830, DE-SC0002623]
- Los Alamos National Laboratory [DE-AC52-06NA25396]
- Northwestern University [NSF DMR-1006069]
- NSF [DMR-1006069]
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The physical and chemical behaviors of materials used in energy storage devices, such as lithium-ion batteries (LIBs), are mainly controlled by an electrochemical process, which normally involves insertion/extraction of ions into/from a host lattice with a concurrent flow of electrons to compensate charge balance. The fundamental physics and chemistry governing the behavior of materials in response to the ions insertion/extraction is not known. Herein, a combination of in situ lithiation experiments and large-scale ab initio molecular dynamics simulations are performed to explore the mechanisms of the electrochemically driven solid-state amorphization in Li-Si systems. We find that local electron-rich condition governs the electrochemically driven solid-state amorphization of Li-Si alloys. This discovery provides the fundamental explanation of why lithium insertion in semiconductor and insulators leads to amorphization, whereas in metals, it leads to a crystalline alloy. The present work correlates electrochemically driven reactions with ion insertion, electron transfer, lattice stability, and phase equilibrium.
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