Theoretical Prediction of the Strong Solvent Effect on Reduced Ethylene Carbonate Ring-Opening and Its Impact on Solid Electrolyte Interphase Evolution

2019 ◽  
Vol 123 (29) ◽  
pp. 17695-17702 ◽  
Author(s):  
Mathew J. Boyer ◽  
Gyeong S. Hwang
Keyword(s):  
Theoretical Prediction ◽  
Solvent Effect ◽  
Solid Electrolyte ◽  
Ring Opening ◽  
Ethylene Carbonate ◽  
Solid Electrolyte Interphase

Molecular dynamics investigation of reduced ethylene carbonate aggregation at the onset of solid electrolyte interphase formation

2019 ◽  
Vol 21 (40) ◽  
pp. 22449-22455 ◽  
Author(s):  
Mathew J. Boyer ◽  
Gyeong S. Hwang
Keyword(s):  
Molecular Dynamics ◽  
Solid Electrolyte ◽  
Ethylene Carbonate ◽  
Solid Electrolyte Interphase ◽  
Reactive Intermediates ◽  
P Concentration

Concentration dependent aggregation of reduced ethylene carbonate through Li+ mediation allows for radical combination reactions between the reactive intermediates to stable products such as ethylene dicarbonate.

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>

Understanding the Surface Film Formation on Si Electrodes in Lithium Secondary Batteries with Atomic Force Microscopy

2020 ◽  
Vol 20 (8) ◽  
pp. 4985-4989
Author(s):  
Hee-Youb Song ◽  
Sung-Su Kim ◽  
Paul Maldonado Nogales ◽  
Soon-Ki Jeong
Keyword(s):  
Atomic Force Microscopy ◽  
Solid Electrolyte ◽  
Electrolyte Solution ◽  
Ethylene Carbonate ◽  
Solid Electrolyte Interphase ◽  
Electrolyte Solutions ◽  
Decomposition Reaction ◽  
Lithium Secondary Batteries ◽  
Force Microscopy ◽  
Atomic Force

The solid electrolyte interphase formation on the negative electrodes of lithium secondary batteries has been considered as one of the principal issues limiting the performance of batteries. Si is an attractive electrode material for improving energy density of lithium secondary batteries because of its high specific theoretical capacity (4200 mAh g−1). However, solid electrolyte interphase formation on Si-based electrodes have not been clearly understood in spite of its significance. Herein, the solid electrolyte interphase formation on Si electrodes in electrolyte solutions containing ethylene carbonate or propylene carbonate was investigated by using in-situ atomic force microscopy. Large and irreversible capacity fade in SiO electrodes was confirmed in both electrolyte solutions through cyclic voltammetry and charge/discharge testing. The in-situ atomic force microscopy results indicated that the decomposition reaction occurred in the ethylene carbonate-based electrolyte solution at a potential of ~0.68 V, while the lithium alloying reaction occurred below 0.25 V during the first reduction process. The decomposition reaction was more vigorous and occurred at a higher potential in the propylene carbonate-based electrolyte solution, resulting in the formation of a thick solid electrolyte interphase film. These results suggest that the solid electrolyte interphase formation on Si electrodes is strongly influenced by the composition of the electrolyte solution.

scholarly journals Model Studies on Solid Electrolyte Interphase Formation on Graphite Electrodes in Ethylene Carbonate and Dimethyl Carbonate II: Graphite Powder Electrodes

2020 ◽  
Vol 7 (23) ◽  
pp. 4794-4809
Author(s):  
Isabella Weber ◽  
Bin Wang ◽  
Carina Bodirsky ◽  
Monalisa Chakraborty ◽  
Mario Wachtler ◽  
...  
Keyword(s):  
Solid Electrolyte ◽  
Dimethyl Carbonate ◽  
Ethylene Carbonate ◽  
Solid Electrolyte Interphase ◽  
Graphite Powder ◽  
Graphite Electrodes ◽  
Model Studies

scholarly journals CO2-based atomic/molecular layer deposition of lithium ethylene carbonate thin films

2020 ◽  
Vol 2 (6) ◽  
pp. 2441-2447
Author(s):  
Juho Heiska ◽  
Milad Madadi ◽  
Maarit Karppinen
Keyword(s):  
Thin Films ◽  
Solid Electrolyte ◽  
Lithium Ion Battery ◽  
Ethylene Carbonate ◽  
Molecular Layer ◽  
Solid Electrolyte Interphase ◽  
Lithium Ion ◽  
Molecular Layer Deposition ◽  
Organic Species ◽  
Layer Deposition

CO2 is used as a precursor in atomic/molecular layer deposition (ALD/MLD) for the fabrication of lithium ethylene carbonates, which are the organic species that naturally form in the solid electrolyte interphase of a typical lithium-ion battery.

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