Advanced Low‐Flammable Electrolytes for Stable Operation of High‐Voltage Lithium‐Ion Batteries

Jia, Hao; Xu, Yaobin; Zhang, Xianhui; Burton, Sarah D.; Gao, Peiyuan; Matthews, Bethany E.; Engelhard, Mark H.; Han, Kee Sung; Zhong, Lirong; Wang, Chongmin; Xu, Wu

doi:10.1002/anie.202102403

Cited by 94 publications

(75 citation statements)

References 22 publications

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“…This dense SEI is considered to be beneficial to the good cycling performance of the electrodes. 50 Figure 7c shows EIS of the Gr||Li cell after 100 cycles in two electrolytes. The diameter of the compressed semicircle indicates two parts, which are SEI and charge transfer.…”

Section: Resultsmentioning

confidence: 99%

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High-Safety and Dendrite-Free Lithium Metal Batteries Enabled by Building a Stable Interface in a Nonflammable Medium-Concentration Phosphate Electrolyte

Zhang

Wei

et al. 2021

ACS Appl. Mater. Interfaces

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Lithium metal anodes are promising for their high energy density and low working potential. However, high reactivity and dendrite growth of lithium metal lead to serious safety issues. Lithium dendrite may form "dead lithium" or pierce the separator, which will cause low efficiency and short-circuit inside the battery. A nonflammable phosphate-based electrolyte can effectively solve the flammability problem. Also, it shows poor compatibility with lithium metal anodes, resulting in an unstable solid electrolyte interface (SEI), which leads to dendrite growth and poor electrochemical performance. In this study, trimethyl phosphate is used to ensure the safety of lithium metal batteries. By adjusting the concentration of lithium salt and introducing fluoroethylene carbonate, a stable SEI layer is formed on the surface of the lithium metal anode and dendrite growth of the lithium metal anode is inhibited. Lithium metal batteries with a modified electrolyte achieved stable electrochemical plating/stripping, and the full cell has 93.4% capacity left and the coulombic efficiency is nearly 100%. In addition, the modified electrolyte can also enable reversible intercalation and de-intercalation of Li + in the commercial graphite anode. This work may provide an alternative direction for the development of lithium metal batteries with high safety and high energy density.

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Section: Resultsmentioning

confidence: 99%

“…As shown in Figure b, in 1.5 M LiFSI/TMP + 5%FEC, even after 100 cycles, a smooth and uniform SEI layer is built on the graphite electrode. This dense SEI is considered to be beneficial to the good cycling performance of the electrodes Figure c shows EIS of the Gr||Li cell after 100 cycles in two electrolytes.…”

Section: Resultsmentioning

confidence: 99%

High-Safety and Dendrite-Free Lithium Metal Batteries Enabled by Building a Stable Interface in a Nonflammable Medium-Concentration Phosphate Electrolyte

Zhang

Wei

et al. 2021

ACS Appl. Mater. Interfaces

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“…Efforts have been made to address the flammability concerns regarding the usage of a liquid electrolyte by discovering other safe alternatives to anions, such as phosphates, borates, imides and Hückel-type salts [ 29 , 30 , 31 , 32 , 33 , 34 , 35 , 36 , 37 ]. Incorporating hydrophilic lithium bis(trifluoromethanesulfonyl)imide, LiTFSI, into the electrolyte system is another strategy as it acts as a co-salt [ 38 , 39 ].…”

Section: Introductionmentioning

confidence: 99%

Ionic Liquid@Metal-Organic Framework as a Solid Electrolyte in a Lithium-Ion Battery: Current Performance and Perspective at Molecular Level

et al. 2022

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Searching for a suitable electrolyte in a lithium-ion battery is a challenging task. The electrolyte must not only be chemically and mechanically stable, but also be able to transport lithium ions efficiently. Ionic liquid incorporated into a metal–organic framework (IL@MOF) has currently emerged as an interesting class of hybrid material that could offer excellent electrochemical properties. However, the understanding of the mechanism and factors that govern its fast ionic conduction is crucial as well. In this review, the characteristics and potential use of IL@MOF as an electrolyte in a lithium-ion battery are highlighted. The importance of computational methods is emphasized as a comprehensive tool to investigate the atomistic behavior of IL@MOF and its interaction in electrochemical environments.

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“…To clarify the interaction between TMP and lithium in the SEI layer, we performed X-ray photoelectron spectroscopy (XPS) on the surface of cycled Li foil. As shown in Figure (a, b), a number of different phosphorus-containing compounds including LiPO 3 and Li 3 PO 4 were detected on the surface of the lithium foil after cycling, indicating that TMP is involved in the formation of SEI and has reacted and has been decomposed. The characteristic species Li 2 CO 3 has also been identified in both the C 1s and O 1s spectrum as shown in Figures S5(a) and (c), respectively .…”

Section: Resultsmentioning

confidence: 96%

Electrochemically-Matched and Nonflammable Janus Solid Electrolyte for Lithium–Metal Batteries

Liu

Wang

et al. 2021

ACS Appl. Mater. Interfaces

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Solid-state batteries based on ceramic electrolytes are promising alternatives to lithium-ion batteries with better safety and energy density. While solid electrolytes such as the garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) are chemically stable with lithium metal, their rigidity leads to poor interfacial contact with the cathodes. Nonflammable organic phosphates, however, are characterized by a liquid nature and can immerse the conventional porous cathodes to form a good contact. However, the phosphates are unstable with lithium metal anodes. We design a quasi-solid Janus electrolyte based on the ceramic LLZO and a trimethyl phosphate (TMP) gel which combines the best of both worlds. The electrochemical window of the Janus electrolyte is significantly extended compared with the TMP to accommodate the lithium metal anode. The contact between the cathode and the electrolyte is maintained by the semifluid nature of the TMP gel. A lithium−metal battery with such a Janus electrolyte can stably cycle at room temperature at 1C while still retaining a capacity of 115 mAh g −1 over 100 times. In contrast, the batteries based on LLZO and TMP individually cannot function properly. More importantly, despite the quasi-solid nature, the battery does not contain flammable functional parts and can alleviate the safety concerns of current batteries containing organic-type electrolytes. This work provides a simple but effective strategy for safe, inexpensive, and energy-dense solid-state batteries.

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Advanced Low‐Flammable Electrolytes for Stable Operation of High‐Voltage Lithium‐Ion Batteries

Cited by 94 publications

References 22 publications

High-Safety and Dendrite-Free Lithium Metal Batteries Enabled by Building a Stable Interface in a Nonflammable Medium-Concentration Phosphate Electrolyte

High-Safety and Dendrite-Free Lithium Metal Batteries Enabled by Building a Stable Interface in a Nonflammable Medium-Concentration Phosphate Electrolyte

Ionic Liquid@Metal-Organic Framework as a Solid Electrolyte in a Lithium-Ion Battery: Current Performance and Perspective at Molecular Level

Electrochemically-Matched and Nonflammable Janus Solid Electrolyte for Lithium–Metal Batteries

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