Probing the morphological influence on solid electrolyte interphase and impedance response in intercalation electrodes

2015 ◽  
Vol 17 (15) ◽  
pp. 9812-9827 ◽  
Author(s):  
Chien-Fan Chen ◽  
Partha P. Mukherjee
Keyword(s):  
Solid Electrolyte ◽  
Solid Electrolyte Interphase ◽  
Active Material ◽  
Impedance Model ◽  
Impedance Response ◽  
Intercalation Electrodes ◽  
The Impact

The microstructure-aware impedance model allows for the impact of active material morphology on the SEI formation and corresponding impedance response.

scholarly journals Li2O-Based Cathode Additives Enabling Prelithiation of Si Anodes

2021 ◽  
Vol 11 (24) ◽  
pp. 12027
Author(s):  
Yeyoung Ha ◽  
Maxwell C. Schulze ◽  
Sarah Frisco ◽  
Stephen E. Trask ◽  
Glenn Teeter ◽  
...  
Keyword(s):  
Coulombic Efficiency ◽  
High Surface ◽  
Solid Electrolyte Interphase ◽  
Active Material ◽  
High Surface Area ◽  
Lithium Ion ◽  
Particle Morphology ◽  
Lithium Oxide ◽  
Si Anodes ◽  
The Impact

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 (Li2O) was added to a LiNi0.6Mn0.2Co0.2O2 (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, Co3O4, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li2O. The Li2O + Co3O4 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.

scholarly journals Leveraging Cation Identity to Engineer Solid Electrolyte Interphases for Rechargeable Lithium Metal Anodes

2020 ◽  
Author(s):  
Richard May ◽  
Yumin Zhang ◽  
Steven R. Denny ◽  
Venkatasubramanian Viswanathan ◽  
Lauren Marbella
Keyword(s):  
Solid Electrolyte ◽  
Density Functional ◽  
Coulombic Efficiency ◽  
Ethylene Carbonate ◽  
Solid Electrolyte Interphase ◽  
Spectroscopic Characterization ◽  
Lithium Metal ◽  
Lithium Metal Anodes ◽  
The Impact ◽  
Metal Anodes

<p>Lithium metal anodes enable substantially higher energy density than current technologies for Li batteries. However, rechargeable Li metal anodes suffer from low Coulombic efficiency (loss of electrochemically active Li), leading to poor cycle life and safety. Engineering the electrolyte formulation to form a stable, well-functioning solid electrolyte interphase (SEI) is a promising approach to improving these performance figures of merit. While design rules have been established for selecting electrolyte solvents and salt anions to establish a more robust SEI, the impact of altering cation identity is not well understood. In this work, we demonstrate that alkali metal additives (here, K<sup>+</sup>) alter SEI composition and thickness. Through post-mortem elemental analyses, we show that K<sup>+</sup> ions do not directly participate in metal electrodeposition, but rather modify the chemical and electrochemical reactivity of the electrode-electrolyte interface. Through a combination of quantitative nuclear magnetic resonance (NMR) spectroscopic characterization and density functional theory (DFT) simulations, we show that decomposition of electrolyte solvent molecules, ethylene carbonate (EC) and dimethyl carbonate (DMC), at the lithium metal surface is suppressed in the presence of a K<sup>+</sup> additive. We attribute this to K<sup>+</sup> being a softer cation compared to Li<sup>+</sup>, leading to preferred pair formation between K<sup>+</sup> and the soft base carbonates, and thus increased salt-solvent coordination. Electrolyte cation engineering is an underexplored strategy to control the SEI, and we believe that the mechanistic understanding and insight developed in this work will spur further investigation of this promising approach.</p>

scholarly journals Al2O3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

2021 ◽  
Vol 9 ◽  
Author(s):  
Emily Sahadeo ◽  
Gary Rubloff ◽  
Sang Bok Lee ◽  
Chuan-Fu Lin
Keyword(s):  
Thin Films ◽  
Solid Electrolyte ◽  
Solid Electrolyte Interphase ◽  
Lithium Ion ◽  
Atomic Layer ◽  
Metal Anode ◽  
Future Design ◽  
Wide Availability ◽  
Protection Layer ◽  
The Impact

Among the many emerging technologies under investigation as alternatives to the successful Lithium-ion battery, the magnesium battery is promising due to the wide availability of magnesium, its high volumetric capacity, and the possibility for safety improvements. One of the largest challenges facing rechargeable magnesium batteries is the formation of a passivation layer at the Mg metal anode interface when reactive species in the electrolyte are reduced at the electrode-electrolyte interface. To control the solid electrolyte interphase in Lithium batteries, protective layers called artificial solid electrolyte interphase (ASEI) layers have been successful in improving Li metal anode performance. The approach of protecting Mg metal anodes from electrolyte degradation has been demonstrated by fewer studies in the literature than Li systems. In this work, we discuss the properties of Al2O3 thin films deposited using atomic layer deposition as an artificial solid electrolyte interphase at the Mg anode. Our results demonstrate that Al2O3 does prevent electrolyte degradation due to the reductive nature of Mg. However, undesirable properties such as defects and layer breakdown lead to Mg growth that causes soft-shorting. The soft-shorting occurs with and without the protection layer, indicating the ALD layer does not prevent it and hinders Al2O3 from being an ideal candidate for a protection layer. Crucial effects of this layer on Mg electrochemistry at the interface were observed, including growth of Mg deposits leading to soft-shorting of the cell whose morphology showed a dependence on the Al2O3 layer. These results may provide guidelines for the future design and development of protective ASEI layers for Mg anodes.

scholarly journals Leveraging Cation Identity to Engineer Solid Electrolyte Interphases for Rechargeable Lithium Metal Anodes

2020 ◽  
Author(s):  
Richard May ◽  
Yumin Zhang ◽  
Steven R. Denny ◽  
Venkatasubramanian Viswanathan ◽  
Lauren Marbella
Keyword(s):  
Solid Electrolyte ◽  
Density Functional ◽  
Coulombic Efficiency ◽  
Ethylene Carbonate ◽  
Solid Electrolyte Interphase ◽  
Spectroscopic Characterization ◽  
Lithium Metal ◽  
Lithium Metal Anodes ◽  
The Impact ◽  
Metal Anodes

<p>Lithium metal anodes enable substantially higher energy density than current technologies for Li batteries. However, rechargeable Li metal anodes suffer from low Coulombic efficiency (loss of electrochemically active Li), leading to poor cycle life and safety. Engineering the electrolyte formulation to form a stable, well-functioning solid electrolyte interphase (SEI) is a promising approach to improving these performance figures of merit. While design rules have been established for selecting electrolyte solvents and salt anions to establish a more robust SEI, the impact of altering cation identity is not well understood. In this work, we demonstrate that alkali metal additives (here, K<sup>+</sup>) alter SEI composition and thickness. Through post-mortem elemental analyses, we show that K<sup>+</sup> ions do not directly participate in metal electrodeposition, but rather modify the chemical and electrochemical reactivity of the electrode-electrolyte interface. Through a combination of quantitative nuclear magnetic resonance (NMR) spectroscopic characterization and density functional theory (DFT) simulations, we show that decomposition of electrolyte solvent molecules, ethylene carbonate (EC) and dimethyl carbonate (DMC), at the lithium metal surface is suppressed in the presence of a K<sup>+</sup> additive. We attribute this to K<sup>+</sup> being a softer cation compared to Li<sup>+</sup>, leading to preferred pair formation between K<sup>+</sup> and the soft base carbonates, and thus increased salt-solvent coordination. Electrolyte cation engineering is an underexplored strategy to control the SEI, and we believe that the mechanistic understanding and insight developed in this work will spur further investigation of this promising approach.</p>

scholarly journals Leveraging Cation Identity to Engineer Solid Electrolyte Interphases for Rechargeable Lithium Metal Anodes

2020 ◽  
Author(s):  
Richard May ◽  
Yumin Zhang ◽  
Steven R. Denny ◽  
Venkatasubramanian Viswanathan ◽  
Lauren Marbella
Keyword(s):  
Solid Electrolyte ◽  
Density Functional ◽  
Coulombic Efficiency ◽  
Ethylene Carbonate ◽  
Solid Electrolyte Interphase ◽  
Spectroscopic Characterization ◽  
Lithium Metal ◽  
Lithium Metal Anodes ◽  
The Impact ◽  
Metal Anodes

<p>Lithium metal anodes enable substantially higher energy density than current technologies for Li batteries. However, rechargeable Li metal anodes suffer from low Coulombic efficiency (loss of electrochemically active Li), leading to poor cycle life and safety. Engineering the electrolyte formulation to form a stable, well-functioning solid electrolyte interphase (SEI) is a promising approach to improving these performance figures of merit. While design rules have been established for selecting electrolyte solvents and salt anions to establish a more robust SEI, the impact of altering cation identity is not well understood. In this work, we demonstrate that alkali metal additives (here, K<sup>+</sup>) alter SEI composition and thickness. Through post-mortem elemental analyses, we show that K<sup>+</sup> ions do not directly participate in metal electrodeposition, but rather modify the chemical and electrochemical reactivity of the electrode-electrolyte interface. Through a combination of quantitative nuclear magnetic resonance (NMR) spectroscopic characterization and density functional theory (DFT) simulations, we show that decomposition of electrolyte solvent molecules, ethylene carbonate (EC) and dimethyl carbonate (DMC), at the lithium metal surface is suppressed in the presence of a K<sup>+</sup> additive. We attribute this to K<sup>+</sup> being a softer cation compared to Li<sup>+</sup>, leading to preferred pair formation between K<sup>+</sup> and the soft base carbonates, and thus increased salt-solvent coordination. Electrolyte cation engineering is an underexplored strategy to control the SEI, and we believe that the mechanistic understanding and insight developed in this work will spur further investigation of this promising approach.</p>

scholarly journals Evolution of solid electrolyte interphase and active material in the silicon wafer model system

2021 ◽  
Vol 482 ◽  
pp. 228946 ◽  
Author(s):  
Caleb Stetson ◽  
Yanli Yin ◽  
Andrew Norman ◽  
Steven P. Harvey ◽  
Manuel Schnabel ◽  
...  
Keyword(s):  
Solid Electrolyte ◽  
Silicon Wafer ◽  
Solid Electrolyte Interphase ◽  
Active Material ◽  
Model System

Unveiling the Formation of Solid Electrolyte Interphase and its Temperature Dependence in “Water-in-Salt” Supercapacitors

2021 ◽  
Vol 13 (3) ◽  
pp. 3979-3990
Author(s):  
Ting Quan ◽  
Eneli Härk ◽  
Yaolin Xu ◽  
Ibbi Ahmet ◽  
Christian Höhn ◽  
...  
Keyword(s):  
Solid Electrolyte ◽  
Temperature Dependence ◽  
Solid Electrolyte Interphase

Reactivity and Evolution of Ionic Phases in the Lithium Solid–Electrolyte Interphase

2021 ◽  
pp. 877-885
Author(s):  
Rui Guo ◽  
Dongniu Wang ◽  
Lucia Zuin ◽  
Betar M. Gallant
Keyword(s):  
Solid Electrolyte ◽  
Solid Electrolyte Interphase
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