High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase

Periyapperuma, Kalani; Arca, Elisabetta; Harvey, Steven; Pathirana, Thushan; Ban, Chunmei; Burrell, Anthony; Pozo-Gonzalo, Cristina; Howlett, Patrick C.

doi:10.1021/acsami.0c09074

High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase

Journal Article · Wed Sep 02 00:00:00 EDT 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c09074· OSTI ID:1665837

^[1]; Arca, Elisabetta ^[2]; ^[2]; Pathirana, Thushan ^[1]; ^[2]; Burrell, Anthony ^[2]; Pozo-Gonzalo, Cristina ^[1]; ^[1]

Deakin Univ., Melbourne, VIC (Australia)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

High-energy-density systems with fast charging rates and suppressed dendrite growth are critical for the implementation of efficient and safe next-generation advanced battery technologies such as those based on Li metal. However, there are few studies that investigate reliable cycling of Li metal electrodes under high-rate conditions. in this work, by employing a superconcentrated ionic liquid (IL) electrolyte, we highlight the effect of Li salt concentration and applied current density on the resulting Li deposit morphology and solid electrolyte interphase (SEI) characteristics, demonstrating exceptional deposition/dissolution rates and efficiency in these systems. Operation at higher current densities enhanced the cycling efficiency, e.g., from 64 ± 3% at 1 mA cm^–2 up to 96 ± 1% at 20 mA cm^–2 (overpotential <±0.2 V), while resulting in lower electrode resistance and dendrite-free Li morphology. A maximum current density of 50 mA cm^–2 resulted in 88 ± 3% cycling efficiency, displaying tolerance for high overpotentials at the Ni working electrode (0.5 V). X-ray photoelectron microscopy (XPS), time-of-flight secondary-ion mass spectroscopy (ToF-SIMS), and scanning electron microscopy (SEM) surface measurements revealed that the formation of a stable SEI, rich in LiF and deficient in organic carbon species, coupled with nondendritic and compact Li morphologies enabled enhanced cycling efficiency at higher currents. Reduced dendrite formation at high current is further highlighted by the use of a highly porous separator in coin cell cycling (1 mAh cm^–2 at 50 °C), sustaining 500 cycles at 10 mA cm^–2.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: Australian Research Council (ARC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1665837

Report Number(s):: NREL/JA--5K00-77342; MainId:26288; UUID:6235ead2-13a4-467a-805f-05520f9f6078; MainAdminID:17447

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 37 Vol. 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase

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