Rejuvenating Propylene Carbonate‐based Electrolyte Through Nonsolvating Interactions for Wide‐Temperature Li‐ions Batteries (Adv. Energy Mater. 48/2022)

Qin, Mingsheng; Liu, Mengchuang; Zeng, Ziqi; Wu, Qiang; Wu, Yuanke; Zhang, Han; Lei, Sheng; Ai, Xiaomeng; Xie, Jia

doi:10.1002/aenm.202270205

Cited by 14 publications

(22 citation statements)

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“…It is believed that the electrochemical behavior of graphite is intimately linked to Li + solvation chemistry and dictated by the formed SEI in LIBs, which inspires two avenues to enable graphite electrode with PC‐dominating electrolyte, namely regulating solvation structure and constructing robust interphase. [ 12–16 ] Indeed, some novel additives, such as Li salts with tailor‐designed structure and new film‐forming molecules, have been tentatively added into PC‐based electrolytes to adjust SEI composition and successfully guaranteed reversible cycling of graphite. [ 17,18 ] Recently, the super‐concentrated electrolytes (SCEs) and diluted SCEs are designed to construct anion‐dominated coordination.…”

Section: Introductionmentioning

confidence: 99%

Revealing Surfactant Effect of Trifluoromethylbenzene in Medium‐Concentrated PC Electrolyte for Advanced Lithium‐Ion Batteries

et al. 2023

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Despite wide‐temperature tolerance and high‐voltage compatibility, employing propylene carbonate (PC) as electrolyte in lithium‐ion batteries (LIBs) is hampered by solvent co‐intercalation and graphite exfoliation due to incompetent solvent‐derived solid electrolyte interphase (SEI). Herein, trifluoromethylbenzene (PhCF3), featuring both specific adsorption and anion attraction, is utilized to regulate the interfacial behaviors and construct anion‐induced SEI at low Li salts’ concentration (<1 m). The adsorbed PhCF3, showing surfactant effect on graphite surface, induces preferential accumulation and facilitated decomposition of bis(fluorosulfonyl)imide anions (FSI−) based on the adsorption–attraction–reduction mechanism. As a result, PhCF3 successfully ameliorates graphite exfoliation‐induced cell failure in PC‐based electrolyte and enables the practical operation of NCM613/graphite pouch cell with high reversibility at 4.35 V (96% capacity retention over 300 cycles at 0.5 C). This work constructs stable anion‐derived SEI at low concentration of Li salt by regulating anions–co‐solvents interaction and electrode/electrolyte interfacial chemistries.

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Section: Introductionmentioning

confidence: 99%

Revealing Surfactant Effect of Trifluoromethylbenzene in Medium‐Concentrated PC Electrolyte for Advanced Lithium‐Ion Batteries

et al. 2023

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“…Seen from Raman spectra, TDSTCN additive can significantly suppress the exfoliation of layered Gr structure at elevated temperature (Figure 4d). [ 50 ] For the first time, we identify that Gr exfoliation at elevated temperature in LiPF 6 ‐carbonate electrolyte (PC‐free) is an important cause of battery capacity loss as well. In‐depth XPS analysis (Ar + sputtering for 0, 20, and 60 nm) of Gr anode clearly reveals that much less Li 2 CO 3 and more LiF is generated with the help of TDSTCN additive (Figure 4e−h).…”

Section: Resultsmentioning

confidence: 99%

Delicately Designed Cyano‐Siloxane as Multifunctional Additive Enabling High Voltage LiNi_0.9Co_0.05Mn_0.05O₂/Graphite Full Cell with Long Cycle Life at 50 °C

Ren

Qiu

Fan

et al. 2023

Adv Funct Materials

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Lithium‐ion batteries (LIBs) adopting layered oxide cathodes with high nickel content (Ni ≥ 0.9) always suffer from extremely poor cycle life, especially at elevated temperatures and higher charging cut‐off voltages. Adding small amounts of functional additives is considered to be one of the most economic and efficacious strategies to resolve this issue. Herein, cyano‐groups are introduced innovatively into a siloxane to delicately synthesize a novel cyano‐siloxane additive, namely 2,2,7,7‐tetramethyl‐3,6‐dioxa‐2,7‐disilaoctane‐4,4,5,5‐tetracarbonitrile (TDSTCN). Encouragingly, 0.5 wt.% TDSTCN additive enables ultrahigh nickel LiNi0.9Co0.05Mn0.05O2/graphite (NCM90/Gr) full cells with dramatically increased cycle life, especially at an elevated temperature of 50 °C and a high charging cut‐off voltage of 4.5 V. The characterizations reveal that the TDSTCN additive can scavenge HF and promote the formation of robust stable interface layers on NCM90 cathode and Gr anode due to the synergistic effects of cyano‐groups and Si−O bonds. These results reveal the great significance of designing one single additive with several functional groups in enhancing the comprehensive electrochemical performances of high Ni LIBs.

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“…Actually, PC is still anticipated to be used as the main solvent of electrolytes for LIBs nowadays, and large amounts of efforts (such as adopting co‐solvents, additives, or lithium salts) have been devoted to deciphering and improving the interphase compatibility between PC‐based electrolytes and graphite anode. [ 25–28,32–43 ] However, to date, the understanding of PC‐induced graphite exfoliation and its suppression mechanism is still not comprehensive. [ 26–28,42,43 ] As a result, the embarrassing situation is that practical high capacity (over 2 Ah) LIBs using PC‐based electrolytes (PC content over 50 vol%, EC‐free) are rarely reported at present.…”

Section: Introductionmentioning

confidence: 99%

Transformed Solvation Structure of Noncoordinating Flame‐Retardant Assisted Propylene Carbonate Enabling High Voltage Li‐Ion Batteries with High Safety and Long Cyclability

Lü

Zhang

et al. 2023

Advanced Energy Materials

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The evolution of high‐energy‐density lithium‐ion batteries (LIBs) urgently requires the development of high‐safety electrolytes with high voltage resistance. Here, noncoordinating flame retardant pentafluoro‐(phenoxy)‐cyclotriphosphazene (FPPN) endows propylene carbonate (PC, 70 vol%)‐based electrolytes with high graphite anode compatibility, non‐flammability, high voltage stability, and excellent separator/electrode wettability. Theoretical calculations reveal that FPPN significantly affects Li+‐PC‐anion interactions and favors Li+ desolvation. Based on in situ optical microscopy and in situ differential electrochemical mass spectrometry, it is innovatively proposed that large amounts of H2 and C3H6 from PC decomposition play a dominant role in destroying the graphitic structure. The evolution of H2 and C3H6 is dramatically alleviated and totally suppressed, respectively, when FPPN prevents PC‐induced graphite exfoliation. More encouragingly, an optimized PC/FPPN‐based electrolyte (70 vol% PC) enables a high voltage LiCoO2/graphite pouch cell (4.35 V, ≈2.6 Ah, ≈242 Wh kg−1) with excellent cycle life and high safety. This work deepens the understanding of PC‐graphite compatibility and opens a new avenue of realizing practical application of PC‐based electrolytes (PC content over 50 vol%) in high capacity (over 2 Ah) LIBs.

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Rejuvenating Propylene Carbonate‐based Electrolyte Through Nonsolvating Interactions for Wide‐Temperature Li‐ions Batteries (Adv. Energy Mater. 48/2022)

Cited by 14 publications

References 0 publications

Revealing Surfactant Effect of Trifluoromethylbenzene in Medium‐Concentrated PC Electrolyte for Advanced Lithium‐Ion Batteries

Revealing Surfactant Effect of Trifluoromethylbenzene in Medium‐Concentrated PC Electrolyte for Advanced Lithium‐Ion Batteries

Delicately Designed Cyano‐Siloxane as Multifunctional Additive Enabling High Voltage LiNi_0.9Co_0.05Mn_0.05O₂/Graphite Full Cell with Long Cycle Life at 50 °C

Transformed Solvation Structure of Noncoordinating Flame‐Retardant Assisted Propylene Carbonate Enabling High Voltage Li‐Ion Batteries with High Safety and Long Cyclability

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Rejuvenating Propylene Carbonate‐based Electrolyte Through Nonsolvating Interactions for Wide‐Temperature Li‐ions Batteries (Adv. Energy Mater. 48/2022)

Cited by 14 publications

References 0 publications

Revealing Surfactant Effect of Trifluoromethylbenzene in Medium‐Concentrated PC Electrolyte for Advanced Lithium‐Ion Batteries

Revealing Surfactant Effect of Trifluoromethylbenzene in Medium‐Concentrated PC Electrolyte for Advanced Lithium‐Ion Batteries

Delicately Designed Cyano‐Siloxane as Multifunctional Additive Enabling High Voltage LiNi0.9Co0.05Mn0.05O2/Graphite Full Cell with Long Cycle Life at 50 °C

Transformed Solvation Structure of Noncoordinating Flame‐Retardant Assisted Propylene Carbonate Enabling High Voltage Li‐Ion Batteries with High Safety and Long Cyclability

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Delicately Designed Cyano‐Siloxane as Multifunctional Additive Enabling High Voltage LiNi_0.9Co_0.05Mn_0.05O₂/Graphite Full Cell with Long Cycle Life at 50 °C