2020/10/31 by Zeeshan Ahmad, Victor Venturi, Hasnain Hafiz +1
Chemistry · Engineering · Medicine · Physics and Astronomy · #Advanced Battery Materials and Technologies #Advanced Battery Technologies Research #Advancements in Battery Materials #Biology #Chemistry #Electrode #Electrolyte #Internal medicine #Interphase #Ion #Lithium (medication) #Lithium metal #Materials science #Medicine #Physical chemistry #cond-mat.mtrl-sci #physics.chem-ph
paper · pdf · doi:10.1021/acs.jpcc.1c00867
published as J. Phys. Chem. C 125, 11301 (2021) · 24 + 6 + 1 pages, 7 figures, 6 pages of Supporting Information. v2: more detailed explanation of defective structure, added references etc
openalex created_date 2020/11/09 · arxiv created 2020/12/04 · openalex publication_date 2021/05/20 · arxiv updated 2021/06/07 · openalex updated_date 2026/08/05
The existence of passivating layers at the interfaces is a major factor enabling modern lithium-ion (Li-ion) batteries. The properties of the passivation layers determine the cycle life, performance, and safety of batteries. One critical passivation layer is the solid electrolyte interphase (SEI), a heterogeneous multicomponent film formed due to the decomposition of the electrolyte at the surface of the anode. The multicomponent nature is critical for its functioning as the interfaces between these components play a critical role in determining performance and safety. In this work, we use first-principles simulations to investigate the thermodynamic, kinetic, and electronic properties of the interface between lithium fluoride (LiF) and lithium carbonate (Li 2 CO 3 ), two common SEI components present in Li-ion batteries with organic liquid electrolytes. We construct a coherent interface between these components that restricts the strain in each of them to below 3%. We find that the interfacial structure has a formation energy of the Frenkel defect higher than bulk calculations and similar to pristine Li 2 CO 3, generating Li vacancies in LiF and Li interstitials in Li 2 CO 3 responsible for transport. On the other hand, the Li interstitial hopping barrier is reduced from 0.3 eV in bulk Li 2 CO 3 to 0.10 or 0.22 eV in the interfacial structure considered, demonstrating the favorable role of the interface. Controlling these two effects in a heterogeneous SEI is crucial for maintaining fast ion transport in the SEI. We further perform Car–Parrinello molecular dynamics simulations to explore Li-ion conduction in our interfacial structure, which reveal an enhanced Li-ion diffusion in the vicinity of the interface. Understanding the interfacial properties of the multiphase SEI represents an important frontier to enable next-generation batteries.