Low-solvation electrolytes for high-voltage sodium-ion batteries

Jin, Yan; Le, Phuong; Gao, Peiyuan; Xu, Yaobin; Xiao, Biwei; Engelhard, Mark H.; Cao, Xia; Võ, Dũng Trung; Hu, Jiangtao; Zhong, Lirong; Matthews, Bethany E.; Yi, Ran; Wang, Chongmin; Li, Xiaolin; Liu, Jun; Zhang, Ji‐Guang

doi:10.1038/s41560-022-01055-0

Cited by 205 publications

(147 citation statements)

References 42 publications

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“…This is because the dielectric constant of TEP and HFE is as low as 12 and 2, respectively, whose values are much lower than that of EC (ε = 89.78) and PC (ε = 66.1) in the carbonate-based electrolyte, thereby showing a low solvation capability to the SEI layer. Note that the SEI formed in this study differs from those formed in the sodium ion battery by employing conventional electrolytes, as the species in the SEI formed in sodium-ion batteries are easier to be dissolved . Thus, the exchanged experiment is reliable and reconfirms the importance of electrolyte stability and the rationality of using the interfacial model to interpret the electrode performance.…”

Section: Design Theme and Electrochemical Performancementioning

confidence: 92%

“…Note that the SEI formed in this study differs from those formed in the sodium ion battery by employing conventional electrolytes, as the species in the SEI formed in sodium-ion batteries are easier to be dissolved. 77 Thus, the exchanged experiment is reliable and reconfirms the importance of electrolyte stability and the rationality of using the interfacial model to interpret the electrode performance.…”

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confidence: 99%

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Dipole–Dipole Interaction Induced Electrolyte Interfacial Model To Stabilize Antimony Anode for High-Safety Lithium-Ion Batteries

Sun

Cao

et al. 2022

ACS Energy Lett.

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Electrolyte plays a vital role in determining battery performances, while the effect of solvent molecular interaction on electrode performances is not fully understood yet. Herein, we present an unrevealed dipole−dipole interaction to show the mechanism of solvent interaction effect on stabilizing the electrolyte for high electrode performances. As a paradigm, a new nonflammable triethyl phosphate (TEP)-based electrolyte is designed to stabilize the bulk alloying anode (e.g., Sb), where an interfacial model is constructed according to the solvation structure induced by the dipole−dipole interaction between TEP and the essential 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (HFE). We demonstrate that the Li + −solvent−anion complexes derived from different solvation structures exhibit different kinetic and electrochemical properties, contributing to varied Sb anode performances in different electrolytes. As a result, a high lithium storage capacity of 656 mAh g −1 , robust rate capacities over 4 A g −1 , and a long lifespan of more than 100 cycles are achieved, which are better than those reported before. This work presents a different insight into understanding electrolyte effects on electrode performances and provides a guideline for electrolyte design to stabilize alloying anodes and beyond in metal-ion batteries.

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Section: Design Theme and Electrochemical Performancementioning

confidence: 92%

mentioning

confidence: 99%

Dipole–Dipole Interaction Induced Electrolyte Interfacial Model To Stabilize Antimony Anode for High-Safety Lithium-Ion Batteries

Sun

Cao

et al. 2022

ACS Energy Lett.

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“…In particular, the formed SEI in these electrolytes is rich in inorganic species (e.g., LiF), which are covered by organic species and not easy to be dissolved. 62,63 The high initial Coulombic efficiency of the Sb@SEI anode after changing the electrolyte is as high as 98.6% in Figure 3b, which value is much higher than 85.2% of pristine Sb in the same kind of electrolyte (i.e., 3.75 M LiFSI/ 0.5 M LiDFOB in DME, Figure 1c). This result directly demonstrates that the SEI could be well-preserved in the exchange experiment.…”

mentioning

confidence: 97%

Discerning Roles of Interfacial Model and Solid Electrolyte Interphase Layer for Stabilizing Antimony Anode in Lithium-Ion Batteries

Sun

Cao

et al. 2022

ACS Materials Lett.

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Electrolyte solvation chemistry has attracted great attention since the recent discovery of its effect on the performances of metal-ion batteries. However, it is challenging to discern its decisive influence from the well-known effect of the solid electrolyte interphase (SEI) layer. This issue becomes more complex upon introducing additives into the electrolyte, as the key role of additives in forming the SEI layer or changing the electrolyte solvation structure also become hard to be discerned. Herein, we design a new dimethyl etherbased electrolyte, and then we unravel the effects of solvation chemistry and the SEI on determining electrode performances, such as the antimony (Sb) anode as a promising example for lithium-ion batteries (LIBs). We find that both the unique solvation structure-derived interfacial model and the SEI are necessary to stabilize the Sb anode. The influences of electrolyte components, particularly the lithium difluoro(oxalato)borate additive, were elucidated for the first time by the dynamic molecular behaviors ranging from solvation structure, interfacial model, to microstructure of the SEI. Finally, extremely high performance of the Sb anode with the capacity of 668 mAh g −1 , high-rate performance over 5 A g −1 , and long cycle life over 100 cycles are obtained, which is superior to that previously reported. This work provides a comprehensive guideline for designing electrolytes via a synergetic approach of solvation structure and the SEI aspects.

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“…According to its chemical formula, NaFTFSI has the advantages of high solubility and admirable compatibility with the Na metal electrode . NaFSI is more compatible with the Na metal electrode than NaTFSI, as reported in the literature, while it is more difficult to dissolve in the DOL solvent compared with NaTFSI. NaFTFSI can be considered as a hybrid of NaTFSI and NaFSI, and it could inherit the advantages of both and avoid their shortcomings at the same time.…”

Section: Resultsmentioning

confidence: 89%

Constructing an In Situ Polymer Electrolyte and a Na-Rich Artificial SEI Layer toward Practical Solid-State Na Metal Batteries

Shuai

Lou

Pei

et al. 2022

ACS Appl. Mater. Interfaces

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Sodium is one of the most promising anode candidates for the beyond-lithium-ion batteries. The development of Na metal batteries with a high energy density, high safety, and low cost is desirable to meet the requirements of both portable and stationary electrical energy storage. However, several problems caused by the unstable Na metal anode and the unsafe liquid electrolyte severely hinder their practical applications. Herein, we report a facile but effective methodology to construct an in situ polymer electrolyte and Na-rich artificial solid-electrolyte interface (SEI) layer concurrently. The obtained integrated Na metal batteries display long cycling life and admirable dynamic performance with total inhibition of dendrites, excellent contact of the cathode/polymer electrolyte, and reduction of side reactions during cycling. The modified Na metal electrode with the in situ polymer electrolyte is stable and dendrite-free in repeated plating/stripping processes with a life span of above 1000 h. Moreover, this method is compatible with different cathodes that demonstrate outstanding electrochemical performance in full cells. We believe that this approach provides a practical solution to solid-state Na metal batteries.

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Low-solvation electrolytes for high-voltage sodium-ion batteries

Cited by 205 publications

References 42 publications

Dipole–Dipole Interaction Induced Electrolyte Interfacial Model To Stabilize Antimony Anode for High-Safety Lithium-Ion Batteries

Dipole–Dipole Interaction Induced Electrolyte Interfacial Model To Stabilize Antimony Anode for High-Safety Lithium-Ion Batteries

Discerning Roles of Interfacial Model and Solid Electrolyte Interphase Layer for Stabilizing Antimony Anode in Lithium-Ion Batteries

Constructing an In Situ Polymer Electrolyte and a Na-Rich Artificial SEI Layer toward Practical Solid-State Na Metal Batteries

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