Non-flammable electrolytes with high salt-to-solvent ratios for Li-ion and Li-metal batteries

Zeng, Ziqi; Vijayakumar, M.; Han, Kee Sung; Jiang, Xiaoyu; Cao, Yuliang; Xiao, Ling; Ai, Xinping; Yang, Hanxi; Zhang, Ji‐Guang; Sushko, Maria L.; Liu, Jun

doi:10.1038/s41560-018-0196-y

Cited by 615 publications

(563 citation statements)

References 52 publications

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“…As shown in Figure S22 (Supporting Information), by incorporating only 2% Al in the ultrahigh-Ni layered oxide (LiNi 0.94 Co 0.06 O 2 ) to give LiNi 0.92 Co 0.06 Al 0.02 O 2 , the capacity retention of full cells significantly increases from 47% to 83% after 1000 cycles. Besides Al doping strategy, the application of the emerging innovative electrolyte system such as high-concentrated electrolyte, [73][74][75] ethylene carbonatefree electrolyte [76,77] is also a prospective direction to stabilize the ultrahigh-Ni layered oxide system. Thus, by incorporating only 2% Al, the cyclability of the ultrahigh-Ni layered oxide could be promoted to a level comparable to that of LiNi 0.8 Co 0.1 Mn 0.1 O 2 .…”

Section: Stabilization Of Ultrahigh-ni Layered Oxidesmentioning

confidence: 99%

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries

Manthiram

2019

Advanced Energy Materials

143

111

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Ultrahigh‐Ni layered oxides hold great promise as high‐energy‐density cathodes at an affordable cost for lithium‐ion batteries, yet their practical application is greatly hampered by the poor cyclability. Herein, by employing LiNi0.94Co0.06O2 as a model cathode in a full‐cell configuration, the interphasial and structural evolution processes of ultrahigh‐Ni layered oxides are systematically investigated over the course of their service life (1500 cycles). By applying advanced analytic techniques (e.g., Li‐isotope labeling, region‐of‐interest method), the dynamic chemical evolution on the cathode surface is revealed with spatial resolution, and the correlation between lattice distortion and cathode surface reactivity is established. Benefiting from in situ X‐ray diffraction (XRD) analysis, the ultrahigh‐Ni layered oxide is demonstrated to undergo dual‐phase reaction mechanisms with huge lattice variation, which leads to a decrease in crystallinity and secondary particle pulverization. Furthermore, the critical impact of cathode surface reaction on the graphite anode–electrolyte interphase (AEI) is revealed at nanometer scale, and a universal chemical/physical evolution process of the AEI is illustrated, for the first time. Finally, the practical viability of ultrahigh‐Ni layered oxides is demonstrated through Al‐doping strategy. This work presents a comprehensive understanding of the structural and interphasial degradation of ultrahigh‐Ni layered oxide cathodes for developing high‐energy‐density lithium‐ion batteries.

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Section: Stabilization Of Ultrahigh-ni Layered Oxidesmentioning

confidence: 99%

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries

Manthiram

2019

Advanced Energy Materials

143

111

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“…It results from the decomposition of electrolyte components (salt ions, solvents molecules, and functional additives), which forms a passivation layer on the surface of electrode materials. [27][28][29][30] Recently, considerable effort has been focused on using high concentration electrolytes to restrain the decomposition of the solvent molecules. A compact, thin, and passivating SEI is necessary to enable the long-term operation of batteries beyond the thermodynamic limits of electrolytes, as is the case for the commercial graphite anode.…”

Section: Introductionmentioning

confidence: 99%

“…The constitution and structure of an SEI, generally including carbonaceous (e.g., (CH 2 OCO 2 Li) 2 , ROCO 2 Li, Li 2 CO 3 , and polycarbonates) and noncarbonaceous (e.g., LiF, Li 2 O, LiOH) components, are dependent on the electrolyte. [27,28,30] However, there are still some disadvantages for the concentrated electrolyte, including precipitation of the Li salts at low temperature, difficulty for wetting cell separators and thick electrodes, and higher cost. The decomposition of solvent molecules is the most common pathway for the formation of the SEI.…”

Section: Introductionmentioning

confidence: 99%

Boosting Superior Lithium Storage Performance of Alloy‐Based Anode Materials via Ultraconformal Sb Coating–Derived Favorable Solid‐Electrolyte Interphase

Xiong

Zhou

et al. 2019

Advanced Energy Materials

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Alloy materials such as Si and Ge are attractive as high‐capacity anodes for rechargeable batteries, but such anodes undergo severe capacity degradation during discharge–charge processes. Compared to the over‐emphasized efforts on the electrode structure design to mitigate the volume changes, understanding and engineering of the solid‐electrolyte interphase (SEI) are significantly lacking. This work demonstrates that modifying the surface of alloy‐based anode materials by building an ultraconformal layer of Sb can significantly enhance their structural and interfacial stability during cycling. Combined experimental and theoretical studies consistently reveal that the ultraconformal Sb layer is dynamically converted to Li3Sb during cycling, which can selectively adsorb and catalytically decompose electrolyte additives to form a robust, thin, and dense LiF‐dominated SEI, and simultaneously restrain the decomposition of electrolyte solvents. Hence, the Sb‐coated porous Ge electrode delivers much higher initial Coulombic efficiency of 85% and higher reversible capacity of 1046 mAh g−1 after 200 cycles at 500 mA g−1, compared to only 72% and 170 mAh g−1 for bare porous Ge. The present finding has indicated that tailoring surface structures of electrode materials is an appealing approach to construct a robust SEI and achieve long‐term cycling stability for alloy‐based anode materials.

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“…It is difficult to presume the appropriate concentration for an HCE when a new solvent system is adopted. Considering that the special properties of HCEs come from the depletion of free solvents and the cations are at least four‐coordinated in electrolytes, the HCEs should have a salt‐to‐solvent molar ratio (MR) of higher than 1 : 4 ,. The 2.55 M NaTFSI/TMP (TMP: trimethyl phosphate), 3.3 M LiFSI/TFEP (TFEP: tris(trifluoroethyl) phosphate), 22 m LiTFSI/H 2 O, and 4.2 M LiTFSI/AN has a salt‐to‐solvent MR of 1 : 2, 1 : 2, 1 : 2.5 and 1 : 1.9, respectively,, supporting the view that using MR instead of molarity to describe HCEs is more appropriate.…”

Section: Highly Concentrated Electrolytesmentioning

confidence: 99%

“…reported a completely nonflammable electrolyte composed of NaTFSI and TMP (1 : 2, molar ratio) for DCBs (Figure a) . In the electrolyte with such a high salt‐to‐solvent MR, most of the TMP molecules are coordinated with cations and their reactivity is essentially diminished ,,. In addition, the anions are preferentially decomposed to construct a compact inorganic SEI film on electrodes, which effectively inhibits the decomposition of TMP solvents ,.…”

Section: Highly Concentrated Electrolytesmentioning

confidence: 99%

Electrolytes for Dual‐Carbon Batteries

Jiang

Luo

Zhong³

et al. 2019

ChemElectroChem

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Dual‐carbon batteries (DCBs) are a promising candidate for smart grid applications, owing to their low cost, high power capability, and environmentally friendly benefits. As an essential component of DCBs, electrolytes not only act as a medium for ion migration during the running of the battery, but also provide active ions to be intercalated into carbon electrodes, exerting significant impacts on the electrochemical performance and safety of the DCB. In this Review, we discuss recent progress in electrolyte research for DCBs, including conventional liquid electrolytes, highly concentrated electrolytes, and gel polymer electrolytes, with a focus on their stability and compatibility with carbon electrodes. Finally, we present perspectives on the current limitations and future research directions of electrolytes for DCBs. Some recommendations for battery evaluation are also offered.

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Non-flammable electrolytes with high salt-to-solvent ratios for Li-ion and Li-metal batteries

Cited by 615 publications

References 52 publications

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries

Boosting Superior Lithium Storage Performance of Alloy‐Based Anode Materials via Ultraconformal Sb Coating–Derived Favorable Solid‐Electrolyte Interphase

Electrolytes for Dual‐Carbon Batteries

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