Li2 O-based cathode additives enabling prelithiation of Si Anodes

Yeyoung Ha; Maxwell C. Schulze; Sarah Frisco; Stephen E. Trask; Glenn Teeter; Nathan R. Neale; Gabriel M. Veith; Christopher S. Johnson

doi:10.3390/app112412027

Li₂ O-based cathode additives enabling prelithiation of Si Anodes

Yeyoung Ha, Maxwell C. Schulze, Sarah Frisco, Stephen E. Trask, Glenn Teeter, Nathan R. Neale, Gabriel M. Veith, Christopher S. Johnson

Energy Storage & Conversion

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

Low first-cycle Coulombic efficiency is especially poor for silicon (Si)-based anodes due to the high surface area of the Si-active material and extensive electrolyte decomposition during the initial cycles forming the solid electrolyte interphase (SEI). Therefore, developing successful prelithiation methods will greatly benefit the development of lithium-ion batteries (LiBs) utilizing Si anodes. In pursuit of this goal, in this study, lithium oxide (Li₂ O) was added to a LiNi_0.6 Mn_0.2 Co_0.2 O₂ (NMC622) cathode using a scalable ball-milling approach to compensate for the initial Li loss at the anode. Different milling conditions were tested to evaluate the impact of particle morphology on the additive performance. In addition, Co₃ O₄, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li₂ O. The Li₂ O + Co₃ O₄ additives successfully delivered an additional capacity of 1116 mAh/g_Li2O when charged up to 4.3 V in half cells and 1035 mAh/g_Li2O when charged up to 4.1 V in full cells using Si anodes.

Original language	English
Article number	12027
Journal	Applied Sciences (Switzerland)
Volume	11
Issue number	24
DOIs	https://doi.org/10.3390/app112412027
State	Published - Dec 1 2021

Funding

This work was authored by the National Renewable Energy Laboratory (NREL), operated by the Alliance for Sustainable Energy, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. Funding provided by the U.S. DOE′ s Vehicle Technologies Office (VTO) under the Silicon Consortium Project directed by Brian Cunningham and managed by Anthony Burrell. The submitted manuscript was created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. DOE Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. A portion of this manuscript was authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. DOE (G.M.V.). The Si electrode used in this manuscript is from Argonne’s Cell Analysis, Modeling and Prototyping (CAMP) Facility, which is fully supported by the DOE VTO. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes. Funding: This work was authored by the National Renewable Energy Laboratory (NREL), operated by the Alliance for Sustainable Energy, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. Funding provided by the U.S. DOE′s Vehicle Technologies Office (VTO) under the Silicon Consortium Project directed by Brian Cunningham and managed by Anthony Burrell. The submitted manuscript was created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. DOE Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. A portion of this manuscript was authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. DOE (G.M.V.). The Si electrode used in this manuscript is from Argonne’s Cell Analysis, Modeling and Prototyping (CAMP) Facility, which is fully supported by the DOE VTO. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes.

Funders	Funder number
DOE VTO
U.S. Government
U.S. Department of Energy	DE-AC36-08GO28308
Argonne National Laboratory
National Renewable Energy Laboratory
Vehicle Technologies Office	DE-AC05-00OR22725, DE-AC02-06CH11357

Keywords

Cathode additives
Cobalt oxide
Lithium oxide
Lithium-ion batteries
Prelithiation
Silicon anodes

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.3390/app112412027

Cite this

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title = "Li2 O-based cathode additives enabling prelithiation of Si Anodes",

abstract = "Low first-cycle Coulombic efficiency is especially poor for silicon (Si)-based anodes due to the high surface area of the Si-active material and extensive electrolyte decomposition during the initial cycles forming the solid electrolyte interphase (SEI). Therefore, developing successful prelithiation methods will greatly benefit the development of lithium-ion batteries (LiBs) utilizing Si anodes. In pursuit of this goal, in this study, lithium oxide (Li2 O) was added to a LiNi0.6 Mn0.2 Co0.2 O2 (NMC622) cathode using a scalable ball-milling approach to compensate for the initial Li loss at the anode. Different milling conditions were tested to evaluate the impact of particle morphology on the additive performance. In addition, Co3 O4, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li2 O. The Li2 O + Co3 O4 additives successfully delivered an additional capacity of 1116 mAh/gLi2O when charged up to 4.3 V in half cells and 1035 mAh/gLi2O when charged up to 4.1 V in full cells using Si anodes.",

keywords = "Cathode additives, Cobalt oxide, Lithium oxide, Lithium-ion batteries, Prelithiation, Silicon anodes",

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AU - Teeter, Glenn

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AU - Veith, Gabriel M.

AU - Johnson, Christopher S.

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N2 - Low first-cycle Coulombic efficiency is especially poor for silicon (Si)-based anodes due to the high surface area of the Si-active material and extensive electrolyte decomposition during the initial cycles forming the solid electrolyte interphase (SEI). Therefore, developing successful prelithiation methods will greatly benefit the development of lithium-ion batteries (LiBs) utilizing Si anodes. In pursuit of this goal, in this study, lithium oxide (Li2 O) was added to a LiNi0.6 Mn0.2 Co0.2 O2 (NMC622) cathode using a scalable ball-milling approach to compensate for the initial Li loss at the anode. Different milling conditions were tested to evaluate the impact of particle morphology on the additive performance. In addition, Co3 O4, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li2 O. The Li2 O + Co3 O4 additives successfully delivered an additional capacity of 1116 mAh/gLi2O when charged up to 4.3 V in half cells and 1035 mAh/gLi2O when charged up to 4.1 V in full cells using Si anodes.

AB - Low first-cycle Coulombic efficiency is especially poor for silicon (Si)-based anodes due to the high surface area of the Si-active material and extensive electrolyte decomposition during the initial cycles forming the solid electrolyte interphase (SEI). Therefore, developing successful prelithiation methods will greatly benefit the development of lithium-ion batteries (LiBs) utilizing Si anodes. In pursuit of this goal, in this study, lithium oxide (Li2 O) was added to a LiNi0.6 Mn0.2 Co0.2 O2 (NMC622) cathode using a scalable ball-milling approach to compensate for the initial Li loss at the anode. Different milling conditions were tested to evaluate the impact of particle morphology on the additive performance. In addition, Co3 O4, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li2 O. The Li2 O + Co3 O4 additives successfully delivered an additional capacity of 1116 mAh/gLi2O when charged up to 4.3 V in half cells and 1035 mAh/gLi2O when charged up to 4.1 V in full cells using Si anodes.

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