Effect of Fluoroethylene Carbonate Additives on the Initial Formation of the Solid Electrolyte Interphase on an Oxygen-Functionalized Graphitic Anode in Lithium-Ion Batteries

Intan, Nadia N.; Pfaendtner, Jim

doi:10.1021/acsami.0c18414

Title: Effect of Fluoroethylene Carbonate Additives on the Initial Formation of the Solid Electrolyte Interphase on an Oxygen-Functionalized Graphitic Anode in Lithium-Ion Batteries

Journal Article · Mon Feb 15 00:00:00 EST 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c18414· OSTI ID:1775254

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Univ. of Washington, Seattle, WA (United States)
Univ. of Washington, Seattle, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

The formation of a solid electrolyte interphase (SEI) at the electrode/electrolyte interface substantially affects the stability and lifetime of lithium-ion batteries (LIBs). One of the methods to improve the lifetime of LIBs is by the inclusion of additive molecules to stabilize the SEI. To understand the effect of additive molecules on the initial stage of SEI formation, in this work we compare the decomposition and oligomerization reactions of a fluoroethylene carbonate (FEC) additive on a range of oxygen-functionalized graphitic anodes to those of an ethylene carbonate (EC) organic electrolyte. A series of density functional theory (DFT) calculations augmented by ab initio molecular dynamics (AIMD) simulations reveal that EC decomposition on an oxygen-functionalized graphitic ($$11\bar{2}0$$) edge facet through a nucleophilic attack on an ethylene carbon site (C_E) of an EC molecule (S2 mechanism) is spontaneous during the initial charging process of LIBs. However, decomposition of EC through a nucleophilic attack on a carbonyl carbon (C_C) site (S1 mechanism) results in alkoxide species regeneration that is responsible for continual oligomerization along the graphitic surface. In contrast, FEC prefers to decompose through an S1 pathway, which does not promote alkoxide regeneration. Including FEC as an additive is thus able to suppress alkoxide regeneration and results in a smaller and thinner SEI layer that is more flexible toward lithium intercalation during the charging/discharging process. In addition, we find that the presence of different oxygen functional groups at the surface of graphite dictates the oligomerization products and the LiF formation mechanism in the SEI.

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Research Organization:: Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019483; AC02-05CH11231

OSTI ID:: 1775254

Journal Information:: ACS Applied Materials and Interfaces, Vol. 13, Issue 7; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
lithium-ion batteries (LIBs)
solid-electrolyte interphase (SEI)
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density functional theory (DFT)
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Title: Effect of Fluoroethylene Carbonate Additives on the Initial Formation of the Solid Electrolyte Interphase on an Oxygen-Functionalized Graphitic Anode in Lithium-Ion Batteries

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