scholarly journals Interphase Control in Lithium Metal Batteries Through Electrolyte Design

2021 ◽  
Author(s):  
Urbi Pal ◽  
Dmitrii Rakov ◽  
Bingyu Lu ◽  
Baharak Sayahpour ◽  
Fangfang Chen ◽  
...  
Keyword(s):  
Ionic Liquid ◽  
High Voltage ◽  
High Performance ◽  
Elevated Temperatures ◽  
Coulombic Efficiency ◽  
Decisive Role ◽  
Cycling Performance ◽  
Lithium Metal ◽  
Ionic Liquid Electrolyte ◽  
Metal Anode

<p>Future rechargeable Li metal batteries (LMBs) require a rational electrolyte design to stabilize</p><p>the interfaces between the electrolyte and both the lithium metal anode and the high voltage</p><p>cathode. This remains the greatest challenge in achieving high cycling performance in</p><p>LMBs. We report an ether-aided ionic liquid electrolyte which offers superior Li metal</p><p>deposition, high voltage (5 V) stability and non-flammability. High performance cycling of</p><p>LiNi0.8Mn0.1Co0.1O2 (4.4 V) and LiNi0.6Mn0.2Co0.2O2 (4.3 V) cells is demonstrated with high</p><p>coulombic efficiency (>99.5%) at room temperature and elevated temperatures, even at high</p><p>practical areal capacity for the latter of 3.8 mAh/cm2 and with a capacity retention of 91% after</p><p>100 cycles. The ether-ionic liquid chemistry enables desirable plated Li microstructures with</p><p>high packing density, minimal ‘dead’ or inactive lithium formation and dendrite-free long-term</p><p>cycling. Along with XPS studies of cycled electrode surfaces, we use molecular dynamics</p><p>simulations to demonstrate that changes to the electrolyte interfacial chemistry upon addition</p><p>of DME plays a decisive role in the formation of a compact stable SEI.</p>

scholarly journals Interphase Control in Lithium Metal Batteries Through Electrolyte Design

2021 ◽  
Author(s):  
Urbi Pal ◽  
Dmitrii Rakov ◽  
Bingyu Lu ◽  
Baharak Sayahpour ◽  
Fangfang Chen ◽  
...  
Keyword(s):  
Ionic Liquid ◽  
High Voltage ◽  
High Performance ◽  
Elevated Temperatures ◽  
Coulombic Efficiency ◽  
Decisive Role ◽  
Cycling Performance ◽  
Lithium Metal ◽  
Ionic Liquid Electrolyte ◽  
Metal Anode

<p>Future rechargeable Li metal batteries (LMBs) require a rational electrolyte design to stabilize</p><p>the interfaces between the electrolyte and both the lithium metal anode and the high voltage</p><p>cathode. This remains the greatest challenge in achieving high cycling performance in</p><p>LMBs. We report an ether-aided ionic liquid electrolyte which offers superior Li metal</p><p>deposition, high voltage (5 V) stability and non-flammability. High performance cycling of</p><p>LiNi0.8Mn0.1Co0.1O2 (4.4 V) and LiNi0.6Mn0.2Co0.2O2 (4.3 V) cells is demonstrated with high</p><p>coulombic efficiency (>99.5%) at room temperature and elevated temperatures, even at high</p><p>practical areal capacity for the latter of 3.8 mAh/cm2 and with a capacity retention of 91% after</p><p>100 cycles. The ether-ionic liquid chemistry enables desirable plated Li microstructures with</p><p>high packing density, minimal ‘dead’ or inactive lithium formation and dendrite-free long-term</p><p>cycling. Along with XPS studies of cycled electrode surfaces, we use molecular dynamics</p><p>simulations to demonstrate that changes to the electrolyte interfacial chemistry upon addition</p><p>of DME plays a decisive role in the formation of a compact stable SEI.</p>

Enhanced Ion Transport in an Ether Aided Super Concentrated Ionic Liquid Electrolyte for Long-Life Practical Lithium Metal Battery Applications

2020 ◽  
Author(s):  
Urbi Pal ◽  
Fangfang Chen ◽  
Derick Gyabang ◽  
Thushan Pathirana ◽  
Binayak Roy ◽  
...  
Keyword(s):  
Ionic Liquid ◽  
Ion Transport ◽  
Current Density ◽  
Coulombic Efficiency ◽  
High Energy ◽  
Liquid Electrolyte ◽  
High Mass ◽  
Lithium Metal ◽  
Ionic Liquid Electrolyte ◽  
Lithium Metal Battery

We explore a novel ether aided superconcentrated ionic liquid electrolyte; a combination of ionic liquid, <i>N</i>-propyl-<i>N</i>-methylpyrrolidinium bis(fluorosulfonyl)imide (C<sub>3</sub>mpyrFSI) and ether solvent, <i>1,2</i> dimethoxy ethane (DME) with 3.2 mol/kg LiFSI salt, which offers an alternative ion-transport mechanism and improves the overall fluidity of the electrolyte. The molecular dynamics (MD) study reveals that the coordination environment of lithium in the ether aided ionic liquid system offers a coexistence of both the ether DME and FSI anion simultaneously and the absence of ‘free’, uncoordinated DME solvent. These structures lead to very fast kinetics and improved current density for lithium deposition-dissolution processes. Hence the electrolyte is used in a lithium metal battery against a high mass loading (~12 mg/cm<sup>2</sup>) LFP cathode which was cycled at a relatively high current rate of 1mA/cm<sup>2</sup> for 350 cycles without capacity fading and offered an overall coulombic efficiency of >99.8 %. Additionally, the rate performance demonstrated that this electrolyte is capable of passing current density as high as 7mA/cm<sup>2</sup> without any electrolytic decomposition and offers a superior capacity retention. We have also demonstrated an ‘anode free’ LFP-Cu cell which was cycled over 50 cycles and achieved an average coulombic efficiency of 98.74%. The coordination chemistry and (electro)chemical understanding as well as the excellent cycling stability collectively leads toward a breakthrough in realizing the practical applicability of this ether aided ionic liquid electrolytes in lithium metal battery applications, while delivering high energy density in a prototype cell.

scholarly journals Ordered LiNi0.5Mn1.5O4 Cathode in Bis(fluorosulfonyl)imide-Based Ionic Liquid Electrolyte: Importance of the Cathode-Electrolyte Interphase

2020 ◽  
Author(s):  
Hyeon Jeong Lee ◽  
Zachary Brown ◽  
Ying Zhao ◽  
Jack Fawdon ◽  
Weixin Song ◽  
...  
Keyword(s):  
Ionic Liquid ◽  
High Voltage ◽  
Rate Capability ◽  
Lithium Ion ◽  
Cycling Performance ◽  
High Energy ◽  
Liquid Electrolyte ◽  
High Energy Density ◽  
X Ray ◽  
Ionic Liquid Electrolyte

<div><div><div><p>The high voltage (4.7 V vs. Li+ /Li) spinel lithium nickel manganese oxide (LiNi0.5 Mn1.5 O4 , LNMO) is a promising candidate for the next-generation of lithium ion batteries due to its high energy density, low cost and environmental impact. However, poor cycling performance at high cutoff potentials limits its commercialization. Herein, hollow structured LNMO is synergistically paired with an ionic liquid electrolyte, 1M lithium bis(fluorosulfonyl)imide (LiFSI) in N-propyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide (Pyr1,3 FSI) to achieve stable cycling performance and improved rate capability. The optimized cathode-electrolyte system exhibits extended cycling performance (>85% capacity retention after 300 cycles) and high rate performance (106.2mAhg–1 at 5C) even at an elevated temperature of 65 ◦C. X-ray photoelectron spectroscopy and spatially resolved x-ray fluorescence analyses confirm the formation of a robust, LiF-rich cathode electrolyte interphase. This study presents a comprehensive design strategy to improve the electrochemical performance of high-voltage cathode materials.</p></div></div></div>

ZnO nanoconfined 3D porous carbon composite microspheres to stabilize lithium nucleation/growth for high-performance lithium metal anodes

2019 ◽  
Vol 7 (33) ◽  
pp. 19442-19452 ◽  
Author(s):  
Linsheng Tang ◽  
Rui Zhang ◽  
Xinyue Zhang ◽  
Naiqin Zhao ◽  
Chunsheng Shi ◽  
...  
Keyword(s):  
Porous Carbon ◽  
High Performance ◽  
Cycling Performance ◽  
Carbon Composite ◽  
Carbon Layer ◽  
Lithium Metal ◽  
Metal Anode ◽  
Composite Microspheres ◽  
Lithium Metal Anode ◽  
Lithium Metal Anodes

The lithiophilic nucleation seed is confined by the carbon layer to improve the cycling performance of the lithium metal anode.

scholarly journals A high-performance potassium metal battery using safe ionic liquid electrolyte

2020 ◽  
Vol 117 (45) ◽  
pp. 27847-27853
Author(s):  
Hao Sun ◽  
Peng Liang ◽  
Guanzhou Zhu ◽  
Wei Hsuan Hung ◽  
Yuan-Yao Li ◽  
...  
Keyword(s):  
Ionic Liquid ◽  
High Performance ◽  
Elevated Temperatures ◽  
High Energy ◽  
Liquid Electrolyte ◽  
Energy Storage Devices ◽  
Ionic Liquid Electrolyte ◽  
Storage Devices ◽  
Safety Issues ◽  
Reduced Graphene

Potassium secondary batteries are contenders of next-generation energy storage devices owing to the much higher abundance of potassium than lithium. However, safety issues and poor cycle life of K metal battery have been key bottlenecks. Here we report an ionic liquid electrolyte comprising 1-ethyl-3-methylimidazolium chloride/AlCl3/KCl/potassium bis(fluorosulfonyl) imide for safe and high-performance batteries. The electrolyte is nonflammable and exhibits a high ionic conductivity of 13.1 mS cm−1at room temperature. A 3.6-V battery with K anode and Prussian blue/reduced graphene oxide cathode delivers a high energy and power density of 381 and 1,350 W kg−1, respectively. The battery shows an excellent cycling stability over 820 cycles, retaining ∼89% of the original capacity with high Coulombic efficiencies of ∼99.9%. High cyclability is also achieved at elevated temperatures up to 60 °C. Uniquely, robust K, Al, F, and Cl-containing passivating interphases are afforded with this electrolyte, which is key to superior battery cycling performances.

Enhanced Ion Transport in an Ether Aided Super Concentrated Ionic Liquid Electrolyte for Long-Life Practical Lithium Metal Battery Applications

2020 ◽  
Author(s):  
Urbi Pal ◽  
Fangfang Chen ◽  
Derick Gyabang ◽  
Thushan Pathirana ◽  
Binayak Roy ◽  
...  
Keyword(s):  
Ionic Liquid ◽  
Ion Transport ◽  
Current Density ◽  
Coulombic Efficiency ◽  
High Energy ◽  
Liquid Electrolyte ◽  
High Mass ◽  
Lithium Metal ◽  
Ionic Liquid Electrolyte ◽  
Lithium Metal Battery

We explore a novel ether aided superconcentrated ionic liquid electrolyte; a combination of ionic liquid, <i>N</i>-propyl-<i>N</i>-methylpyrrolidinium bis(fluorosulfonyl)imide (C<sub>3</sub>mpyrFSI) and ether solvent, <i>1,2</i> dimethoxy ethane (DME) with 3.2 mol/kg LiFSI salt, which offers an alternative ion-transport mechanism and improves the overall fluidity of the electrolyte. The molecular dynamics (MD) study reveals that the coordination environment of lithium in the ether aided ionic liquid system offers a coexistence of both the ether DME and FSI anion simultaneously and the absence of ‘free’, uncoordinated DME solvent. These structures lead to very fast kinetics and improved current density for lithium deposition-dissolution processes. Hence the electrolyte is used in a lithium metal battery against a high mass loading (~12 mg/cm<sup>2</sup>) LFP cathode which was cycled at a relatively high current rate of 1mA/cm<sup>2</sup> for 350 cycles without capacity fading and offered an overall coulombic efficiency of >99.8 %. Additionally, the rate performance demonstrated that this electrolyte is capable of passing current density as high as 7mA/cm<sup>2</sup> without any electrolytic decomposition and offers a superior capacity retention. We have also demonstrated an ‘anode free’ LFP-Cu cell which was cycled over 50 cycles and achieved an average coulombic efficiency of 98.74%. The coordination chemistry and (electro)chemical understanding as well as the excellent cycling stability collectively leads toward a breakthrough in realizing the practical applicability of this ether aided ionic liquid electrolytes in lithium metal battery applications, while delivering high energy density in a prototype cell.

scholarly journals Ordered LiNi0.5Mn1.5O4 Cathode in Bis(fluorosulfonyl)imide-Based Ionic Liquid Electrolyte: Importance of the Cathode-Electrolyte Interphase

2020 ◽  
Author(s):  
Hyeon Jeong Lee ◽  
Zachary Brown ◽  
Ying Zhao ◽  
Jack Fawdon ◽  
Weixin Song ◽  
...  
Keyword(s):  
Ionic Liquid ◽  
High Voltage ◽  
Rate Capability ◽  
Lithium Ion ◽  
Cycling Performance ◽  
High Energy ◽  
Liquid Electrolyte ◽  
High Energy Density ◽  
X Ray ◽  
Ionic Liquid Electrolyte

<div><div><div><p>The high voltage (4.7 V vs. Li+ /Li) spinel lithium nickel manganese oxide (LiNi0.5 Mn1.5 O4 , LNMO) is a promising candidate for the next-generation of lithium ion batteries due to its high energy density, low cost and environmental impact. However, poor cycling performance at high cutoff potentials limits its commercialization. Herein, hollow structured LNMO is synergistically paired with an ionic liquid electrolyte, 1M lithium bis(fluorosulfonyl)imide (LiFSI) in N-propyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide (Pyr1,3 FSI) to achieve stable cycling performance and improved rate capability. The optimized cathode-electrolyte system exhibits extended cycling performance (>85% capacity retention after 300 cycles) and high rate performance (106.2mAhg–1 at 5C) even at an elevated temperature of 65 ◦C. X-ray photoelectron spectroscopy and spatially resolved x-ray fluorescence analyses confirm the formation of a robust, LiF-rich cathode electrolyte interphase. This study presents a comprehensive design strategy to improve the electrochemical performance of high-voltage cathode materials.</p></div></div></div>

scholarly journals Passivation of Lithium Metal Anode via Hybrid Ionic Liquid Electrolyte toward Stable Li Plating/Stripping

2016 ◽  
Vol 4 (2) ◽  
pp. 1600400 ◽  
Author(s):  
Nian-Wu Li ◽  
Ya-Xia Yin ◽  
Jin-Yi Li ◽  
Chang-Huan Zhang ◽  
Yu-Guo Guo
Keyword(s):  
Ionic Liquid ◽  
Liquid Electrolyte ◽  
Lithium Metal ◽  
Ionic Liquid Electrolyte ◽  
Metal Anode ◽  
Lithium Metal Anode

scholarly journals Dendrite-Free and Stable Lithium Metal Battery Achieved by a Model of Stepwise Lithium Deposition and Stripping

2021 ◽  
Vol 13 (1) ◽  
Author(s):  
Tiancun Liu ◽  
Jinlong Wang ◽  
Yi Xu ◽  
Yifan Zhang ◽  
Yong Wang
Keyword(s):  
Reduction Method ◽  
Coulombic Efficiency ◽  
List Type ◽  
Lithium Metal ◽  
Metal Anode ◽  
In Situ Raman ◽  
Unique Model ◽  
Li Metal Anode ◽  
Pyridinic N

Highlights A facile method is adopted to obtain cucumber-like lithiophilic composite skeleton. Massive lithiophilic sites in cucumber-like lithiophilic composite skeleton can promote and guide uniform Li depositions. A unique model of stepwise Li deposition and stripping is determined. Abstract The uncontrolled formation of lithium (Li) dendrites and the unnecessary consumption of electrolyte during the Li plating/stripping process have been major obstacles in developing safe and stable Li metal batteries. Herein, we report a cucumber-like lithiophilic composite skeleton (CLCS) fabricated through a facile oxidation-immersion-reduction method. The stepwise Li deposition and stripping, determined using in situ Raman spectra during the galvanostatic Li charging/discharging process, promote the formation of a dendrite-free Li metal anode. Furthermore, numerous pyridinic N, pyrrolic N, and CuxN sites with excellent lithiophilicity work synergistically to distribute Li ions and suppress the formation of Li dendrites. Owing to these advantages, cells based on CLCS exhibit a high Coulombic efficiency of 97.3% for 700 cycles and an improved lifespan of 2000 h for symmetric cells. The full cells assembled with LiFePO4 (LFP), SeS2 cathodes and CLCS@Li anodes demonstrate high capacities of 110.1 mAh g−1 after 600 cycles at 0.2 A g−1 in CLCS@Li|LFP and 491.8 mAh g−1 after 500 cycles at 1 A g−1 in CLCS@Li|SeS2. The unique design of CLCS may accelerate the application of Li metal anodes in commercial Li metal batteries.

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