Non-flammable fluorobenzene-diluted highly concentrated electrolytes enable high-performance Li-metal and Li-ion batteries

Liu, Mengchuang; Zeng, Ziqi; Zhong, Wei; Ge, Zicheng; Li, Longqing; Lei, Sheng; Wu, Qiang; Zhang, Han; Cheng, Shijie; Xie, Jia

doi:10.1016/j.jcis.2022.03.133

Cited by 21 publications

(9 citation statements)

References 44 publications

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“…Despite FB being highly flammable, the safety can be substantially improved by adding fireretardant additives. [124,125] Moreover, the safety of batteries can be further improved via employing functional separators [126] and advanced battery management system. [127] Commonly adopted binary solutions typically failed at subzero environment because of the drastic drop in conductivity, which calls for additional cosolvents with lower viscosity and high dielectric constant.…”

Section: Carbonate-based Solventmentioning

confidence: 99%

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Challenges and strategies of formulating low‐temperature electrolytes in lithium‐ion batteries

Qin

Zeng

Cheng

et al. 2023

Interdisciplinary Materials

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Lithium-ion batteries (LIBs) have monopolized energy storage markets in modern society. The reliable operation of LIBs at cold condition (<0°C), nevertheless, is inevitably hampered by the sluggish kinetics and parasite reactions, which falls behind the increasing demands for portable electronics and electric vehicles. The electrolyte controls both Li + transport and interfacial reaction, dictating the low-temperature performance substantially. Therefore, the rational formulation of electrolytes is significant for realizing superior lowtemperature performance and broadening application niches of LIBs. Herein, we first discuss the kinetic limitations of low-temperature LIBs, highlighting the importance of electrolyte structure and interfacial chemistry. Then, the advancements for formulating subzero-temperature electrolyte are summarized with in-depth discussions about electrolyte formulation, solvation structure, interfacial chemistry, and low-temperature behaviors. Moreover, some opportunities for lithium metal batteries and the corresponding lowtemperature electrolyte are covered. Finally, the major challenges and future perspectives are outlined for low-temperature LIBs.

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Section: Carbonate-based Solventmentioning

confidence: 99%

“…Despite FB being highly flammable, the safety can be substantially improved by adding fire‐retardant additives. [ 124,125 ] Moreover, the safety of batteries can be further improved via employing functional separators [ 126 ] and advanced battery management system. [ 127 ]…”

Section: Formulating Low‐temperature Electrolytementioning

confidence: 99%

Challenges and strategies of formulating low‐temperature electrolytes in lithium‐ion batteries

Qin

Zeng

Cheng

et al. 2023

Interdisciplinary Materials

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“…[2] Efforts include the utilization of solidpolymer electrolytes, ionic liquids, localized highly concentrated Li salts, and flame-resistant additives to solve such issues. [3] However, Li-ion transport via chain segment motion and high crystallinity in solid polymer electrolytes (SPEs) follow poor ion conduction at ambient temperature. Therefore, for highly safe solid-state polymer electrolytes, low conductivity, and unstable interfacial issues exist for battery operation at low temperatures.…”

Section: Introductionmentioning

confidence: 99%

Transitioning Towards Asymmetric Gel Polymer Electrolytes for Lithium Batteries: Progress and Prospects

Agnihotri,

Ahmed,

Tamilarasan

et al. 2023

Adv Funct Materials

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The utilization of liquid electrolytes (LEs) concerns inevitable dendrite growth and safety issues. In contrast, solid polymer electrolytes suffer from unsettled low ionic conductivity and interfacial impedance issues. The intermediary gel polymer electrolytes (GPEs) improve safety by incorporating a sturdy polymer matrix and ionic conductivity as an advantage of percolating LEs responsible for gelation. The overall stability and compatibility of GPEs with different electrode materials depend on the polymers, plasticizers, and precursors utilized. No single polymer has a wide energy gap to exhibit stability against Li metal anodes and oxidative stability against high‐voltage cathodes. Thereafter, symmetric GPEs (SGPEs) possess limitations while simultaneously satisfying the two electrode requirements, which hinders their practical applications. Asymmetric GPEs (ASGPEs) generally comprise a bilayer or gradient structure, wherein the side contacting the cathode is modified to promote oxidative stability for a stable cathode electrolyte interface (CEI). The corresponding side in contact with the anode is modified to be mechanically and chemically compatible with dendritic lithium. Overall, asymmetric structural engineering enables electrode compatibility while maintaining the physical competency of GPEs. Herein, the focus is to summarize the current transition from SGPEs to asymmetric ones, which promotes multifunctionality while overcoming specific constraints associated with the electrodes.

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“…Considering the intrinsic advantages of carbonate-based electrolytes including low cost and high ionic conductivity, the incorporation of functional co-solvents with flame-retardancy into electrolytes to reduce its flammability is regarded as a keenly anticipated strategy. − Among the reported flame retardants (FRs), phosphate esters represented by triethyl phosphate (TEP) and trimethyl phosphate (TMP) show unrivaled advantages over other FRs, such as low cost, excellent flame-retardancy, and good miscibility with carbonate-based electrolytes. ,,− Unfortunately, once TEP or TMP content in electrolytes reaches the threshold (>40 wt %) required for ensuring electrolyte’s nonflammability, − the solid-state electrolyte interface (SEI) ingredients on the Gr electrode transforms from decomposition products of ethylene carbonate (EC) to those of TEP/TMP. , Due to the poor electronic shielding ability of these products, the Li + -solvents’ co-intercalation or persistent decomposition of solvent are difficult to be prevented; − thus, the Gr electrodes inevitably experience rapid failure.…”

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confidence: 99%

“…At this moment, TEP/TMP re-enters into PSS and reverts to its irreversible decomposition, which leads to the failure of Gr electrodes in the post-cycling process. In addition, it is worth emphasizing that as a class of weakly polar solvents (Figure S1), TEP or TMP demonstrates poor dissociation ability to lithium salts, therefore, upon taking them as main solvents, it is difficult to develop electrolytes with high ionic conductivity. ,,,− Inspired by these studies, controlling TEP/TMP’s number in PSS and establishing a dynamically stable PSS structure in carbonate-based electrolytes are the keys to conferring its excellent stability toward Gr electrodes and high ionic conductivity for TEP/TMP-based nonflammable electrolytes (Schematic , our design). Fortunately, it is possible for carbonate-based electrolytes to accomplish this design for the following reasons: First, the strong coordination of ethylene carbonate (EC) to Li + allows it to compete with TEP/TMP in forming PSS.…”

mentioning

confidence: 99%

Ethylene Carbonate Regulated Solvation of Triethyl Phosphate to Enable High-Conductivity, Nonflammable, and Graphite Compatible Electrolyte

Liu,

Zeng,

et al. 2023

ACS Energy Lett.

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In the landscape of lithium-ion batteries (LIBs), carbonate-based electrolytes have driven remarkable progress, but persistent safety concerns stemming from their flammability necessitate innovative solutions. This study explores a cost-effective nonflammable cosolvent, triethyl phosphate (TEP), to counter the risk. However, TEP's strong Li + -coordinating propensity adversely affects graphite (Gr) electrode intercalation. To surmount these challenges, we unveil the competitive coordination behavior of TEP and ethylene carbonate, strategically optimizing TEP's coordination numbers. This tailored approach culminates in a dynamically stable structure which reduces the adverse effects of TEP. Leveraging these insights, we engineer a TEP-modified carbonate electrolyte with standard Li salt concentration (1 M) boasting both nonflammability and high ionic conductivity, enabling the Gr anode to achieve ∼100% capacity retention after 150 cycles. Additionally, this formulation significantly minimizes fire and explosion risks in 4 A h Gr||LiNi 0.9 Co 0.05 Mn 0.05 O 2 pouch cells during mechanical stress, demonstrating profound implications for safer energy storage in LIBs.

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Non-flammable fluorobenzene-diluted highly concentrated electrolytes enable high-performance Li-metal and Li-ion batteries

Cited by 21 publications

References 44 publications

Challenges and strategies of formulating low‐temperature electrolytes in lithium‐ion batteries

Challenges and strategies of formulating low‐temperature electrolytes in lithium‐ion batteries

Transitioning Towards Asymmetric Gel Polymer Electrolytes for Lithium Batteries: Progress and Prospects

Ethylene Carbonate Regulated Solvation of Triethyl Phosphate to Enable High-Conductivity, Nonflammable, and Graphite Compatible Electrolyte

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