Monolithic heterojunction quasi-solid-state battery electrolytes based on thermodynamically immiscible dual phases

Cho, Sung Ju; Jung, Gwan Yeong; Kim, Su Hwan; Jang, Moongyu; Yang, Doo Kyung; Kwak, Sang Kyu; Lee, Sang Young

doi:10.1039/c8ee01503a

“…10 , we assembled the CIBs using desodiated NVPF cathode, calciated graphite anode in a dual phase liquid electrolyte at room temperature. Since the use of graphite anode in CIB requires the specific choice of electrolyte system for the co-intercalation 15 , the dual phase electrolyte was designed in regard to immiscibility of two liquid phases 47 and chemical compatibility between active material and electrolyte. An all-intercalation-based full cell showed the reversible capacity retention of 63% over 50 cycles, showing the promise of NVPF cathode in diverse cell configurations.…”

Section: Resultsmentioning

confidence: 99%

A new high-voltage calcium intercalation host for ultra-stable and high-power calcium rechargeable batteries

Xu

¹

,

Park

²

,

Wang

³

et al. 2021

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Rechargeable calcium batteries have attracted increasing attention as promising multivalent ion battery systems due to the high abundance of calcium. However, the development has been hampered by the lack of suitable cathodes to accommodate the large and divalent Ca2+ ions at a high redox potential with sufficiently fast ionic conduction. Herein, we report a new intercalation host which presents 500 cycles with a capacity retention of 90% and a remarkable power capability at ~3.2 V (vs. Ca/Ca2+) in a calcium battery. The cathode material derived from Na0.5VPO4.8F0.7 is demonstrated to reversibly accommodate a large amount of Ca2+ ions, forming a series of CaxNa0.5VPO4.8F0.7 (0 < x < 0.5) phases without any noticeable structural degradation. The robust framework enables one of the smallest volume changes (1.4%) and the lowest diffusion barriers for Ca2+ among the cathodes reported to date, offering the basis for the outstanding cycle life and power capability.

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“…Determined from Equation (S1) (Supporting Information), the shuttle factor (f)w as introduced to reflect the degree of the LiPS shuttle effect on Coulombic efficiency,and this effect can be estimated with Equation (S2) (Supporting Information). [38][39][40] The f values of the HFE-based electrolyte are much smaller than those of regular ethers at the same discharge capacity ( Table 1). Thes huttle factor displayed by the electrolyte containing the highly bulky MtBE cosolvent (0.44) is still significantly larger than that of the BTFE-based electrolyte (0.27).…”

Section: Angewandte Chemiementioning

confidence: 96%

A Selection Rule for Hydrofluoroether Electrolyte Cosolvent: Establishing a Linear Free‐Energy Relationship in Lithium–Sulfur Batteries

Su

¹

,

He

²

,

Amine

³

et al. 2019

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Hydrofluoroethers (HFEs) have been adopted widely as electrolyte cosolvents for battery systems because of their unique low solvating behavior.The electrolyte is currently utilized in lithium-ion, lithium-sulfur,lithium-air,and sodiumion batteries.B ye valuating the relative solvating power of different HFEs with distinct structural features,a nd considering the shuttle factor displayed by electrolytes that employ HFE cosolvents,w eh ave established the quantitative structureactivity relationship between the organic structure and the electrochemical performance of the HFEs.Moreover,wehave established the linear free-energy relationship between the structural properties of the electrolyte cosolvents and the polysulfide shuttle effect in lithium-sulfur batteries.T hese findings providev aluable mechanistic insight into the polysulfide shuttle effect in lithium-sulfur batteries,a nd are instructive when it comes to selecting the most suitable HFE electrolyte cosolvent for different battery systems.Over the past few decades,lithium-ion batteries have been applied extensively in consumer electronic devices owing to their relatively high energy density and operating voltage. [1][2][3] To meet the demands of electric vehicle applications, however, the energy density of state-of-the-art lithium batteries must be increased substantially. [4][5][6] Va rious new lithium-battery systems with high theoretical energy density have been proposed. [5][6][7] Fort hese new battery systems to be successful, it is critical to develop reliable electrolytes and to understand their working principles. [8,9] First introduced as an electrolyte cosolvent ad ecade ago, [10] hydrofluoroethers (HFEs) have rapidly been employed by researchers all over the world to construct functional electrolytes for high-voltage lithium-ion, [10][11][12] lithium-metal, [13] lithium-sulfur (Li-S), [14] lithium-air, [15,16] lithium/selenium-sulfur, [17] and even sodium-ion batteries. [18,19] Because of their low solvating ability,H FEs are exceptionally versatile as electrolyte cosolvents.T hey offer several important advantages: 1) enhanced oxidative stability of electrolytes, [10][11][12] 2) they serve as excellent thinning reagents for reducing the viscosity of electrolytes, [20][21][22] and 3) they enable the construction of localized concentrated electrolytes,which are highly useful in lithium-metal batteries. [13,[23][24][25] Significantly,they have gained popularity in Li-S batteries because of their effectiveness in suppressing the lithium polysulfides (LiPS) shuttle effect. [26][27][28][29][30][31][32][33][34] Despite the extensive application of HFEs,t he effect of their intricate molecular structure on electrochemical behavior has hardly been studied. By comparing the electrochemical properties of four HFEs,Shin and co-workers concluded that the degree of fluorination (that is,the number of fluorine atoms) dictated the solvation behavior. [21,35] Yet, it is critical to also consider the position of the fluoroalkyl groups in the HFE structures when e...

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“…The Coulombic efficiencies of the test cells at a specific discharge capacity of 850 mAh g −1 , and the corresponding shuttle factors, are shown in Table . Determined from Equation (S1) (Supporting Information), the shuttle factor ( f ) was introduced to reflect the degree of the LiPS shuttle effect on Coulombic efficiency, and this effect can be estimated with Equation (S2) (Supporting Information) . The f values of the HFE‐based electrolyte are much smaller than those of regular ethers at the same discharge capacity (Table ).…”

Section: Figurementioning

confidence: 99%

A Selection Rule for Hydrofluoroether Electrolyte Cosolvent: Establishing a Linear Free‐Energy Relationship in Lithium–Sulfur Batteries

Su

¹

,

He

²

,

Amine

³

et al. 2019

View full text Add to dashboard Cite

Hydrofluoroethers (HFEs) have been adopted widely as electrolyte cosolvents for battery systems because of their unique low solvating behavior. The electrolyte is currently utilized in lithium‐ion, lithium–sulfur, lithium–air, and sodium‐ion batteries. By evaluating the relative solvating power of different HFEs with distinct structural features, and considering the shuttle factor displayed by electrolytes that employ HFE cosolvents, we have established the quantitative structure–activity relationship between the organic structure and the electrochemical performance of the HFEs. Moreover, we have established the linear free‐energy relationship between the structural properties of the electrolyte cosolvents and the polysulfide shuttle effect in lithium–sulfur batteries. These findings provide valuable mechanistic insight into the polysulfide shuttle effect in lithium–sulfur batteries, and are instructive when it comes to selecting the most suitable HFE electrolyte cosolvent for different battery systems.

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Monolithic heterojunction quasi-solid-state battery electrolytes based on thermodynamically immiscible dual phases

Abstract: Monolithic heterojunction quasi-solid-state battery electrolytes (MH-QEs) based on thermodynamically immiscible dual phases are presented as an electrode-customized multifunctional electrolyte.

Cited by 30 publications

References 41 publications

A new high-voltage calcium intercalation host for ultra-stable and high-power calcium rechargeable batteries

A new high-voltage calcium intercalation host for ultra-stable and high-power calcium rechargeable batteries

A Selection Rule for Hydrofluoroether Electrolyte Cosolvent: Establishing a Linear Free‐Energy Relationship in Lithium–Sulfur Batteries

A Selection Rule for Hydrofluoroether Electrolyte Cosolvent: Establishing a Linear Free‐Energy Relationship in Lithium–Sulfur Batteries

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