Robust Solid/Electrolyte Interphase (SEI) Formation on Si Anodes Using Glyme-Based Electrolytes

Yang, Guang; Frisco, Sarah; Tao, Runming; Philip, Nathan; Bennett, Tyler H.; Stetson, Caleb; Zhang, Ji-Guang; Han, Sang-Don; Teeter, Glenn; Harvey, Steven P.; Zhang, Yunya; Veith, Gabriel M.; Nanda, Jagjit

doi:10.1021/acsenergylett.0c02629

Title: Robust Solid/Electrolyte Interphase (SEI) Formation on Si Anodes Using Glyme-Based Electrolytes

Journal Article · Mon Apr 05 00:00:00 EDT 2021 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.0c02629· OSTI ID:1785091

^[1]; Frisco, Sarah ^[2]; Tao, Runming ^[3]; Philip, Nathan ^[1];

^[1];

^[2];

^[4];

^[2]; Teeter, Glenn ^[2];

^[2]; Zhang, Yunya ^[5];

^[1];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States) ; Univ. of Tennessee, Knoxville, TN (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Silicon (Si) is the most naturally abundant element possessing 10-fold greater theoretical capacity compared to that of graphite-based anodes. The practicality of implementing Si anodes is, however, limited by the unstable solid/electrolyte interphase (SEI) and anode fracturing during continuous lithiation/delithiation. We demonstrate that glyme-based electrolytes (GlyEls) ensure a conformal SEI on Si and keep the Si “fracture-free”. Benchmarking against the optimal, commonly used carbonate electrolyte with the fluoroethylene carbonate additive, the Si anode cycled in a GlyEl exhibits a reduced early parasitic current (by 62.5%) and interfacial resistance (by 72.8%), while cell capacity retention is promoted by >7% over the course of 110 cycles. A mechanistic investigation by X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy indicates GlyEl enriches Si SEI with elastic polyether but diminishes its carbonate species. Glyme-based electrolytes proved to be viable in stabilizing the SEI on Si for future high energy density lithium-ion batteries.

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Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC36-08GO28308; AC05-00OR22725

OSTI ID:: 1785091

Alternate ID(s):: OSTI ID: 1797645

Report Number(s):: NREL/JA-5K00-80105; MainId:42308; UUID:cb172aaa-621c-4240-9ef3-6db81d1e2d84; MainAdminID:24514

Journal Information:: ACS Energy Letters, Vol. 6, Issue 5; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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