Non‐Flammable Electrolyte Enables High‐Voltage and Wide‐Temperature Lithium‐Ion Batteries with Fast Charging

Zou, Yeguo; Ma, Zheng; Liu, Gang; Li, Qian; Yin, Dongming; Shi, Xuejian; Cao, Zhen; Tian, Zhengnan; Kim, Hun; Guo, Yingjun; Sun, Chunsheng; Cavallo, Luigi; Wang, Limin; Alshareef, Husam N.; Sun, Yang‐Kook; Ming, Jun

doi:10.1002/anie.202216189

Cited by 96 publications

(53 citation statements)

References 59 publications

(10 reference statements)

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“…were changed in different battery systems. Thus, our discovery may provide a new challenging direction which is to quantify the solvent–solvent interaction. − We believe more advanced techniques and simulations need to be developed to realize it, by which a certain critical value that the interaction intensity should surpass to stabilize the electrolytes could be estimated.…”

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Weak Solvent–Solvent Interaction Enables High Stability of Battery Electrolyte

Wang

Cao

et al. 2023

ACS Energy Lett.

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Electrolytes play an important role in transporting metal ions (e.g., Li+) in metal ion batteries, while understanding the relationship between the electrolyte properties and behaviors is still challenging. Herein, we detect the existence of weak solvent–solvent interactions in electrolytes by nuclear magnetic resonance (NMR), particularly discovering that such interactions have a significant function of stabilizing the electrolytes, which has never been reported before. As a paradigm, we renovated the understanding of the role of ethylene carbonate (EC) solvent in the lithium-ion battery electrolyte. We find that the EC solvent can stabilize the linear carbonate solvent electrolyte, particularly the diethyl carbonate (DEC) electrolyte, by the weak intermolecular interactions, enhancing the energy difference between the orbitals of the Li+(EC) x (DEC) y complex, in turn demonstrating strong capability against reduction. Our viewpoint was further demonstrated in other metal ion batteries (e.g., Na+, K+), whose discovery is significant for designing electrolytes and in-depth understanding of the battery performance.

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confidence: 99%

Weak Solvent–Solvent Interaction Enables High Stability of Battery Electrolyte

Wang

Cao

et al. 2023

ACS Energy Lett.

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“…− anion locate at ≈843 cm −1 . [21] We find that the proportion of CIPs in FE and FEP electrolytes is higher than that in ED electrolytes. Moreover, the CIPs were also clearly observed at ≈742 cm −1 in FE and FEP electrolytes but disappear in ED electrolytes (Figure 2c).…”

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confidence: 65%

“…[ 20 ] The engagement state of PF 6 − can be also analyzed by the FTIR spectra in the 920–800 cm −1 range (Figure 2b), where the contact ion pairs (CIPs, i.e., Li + ‐solvent‐PF 6 − ) are located at 862–858 and 832–825 cm −1 bands, and the free PF 6 − anion locate at ≈843 cm −1 . [ 21 ] We find that the proportion of CIPs in FE and FEP electrolytes is higher than that in ED electrolytes. Moreover, the CIPs were also clearly observed at ≈742 cm −1 in FE and FEP electrolytes but disappear in ED electrolytes (Figure 2c).…”

Section: Resultsmentioning

confidence: 90%

Intermolecular Interactions Mediated Nonflammable Electrolyte for High‐Voltage Lithium Metal Batteries in Wide Temperature

Zou

Liu

Wang

et al. 2023

Advanced Energy Materials

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limited by the specific capacity of the electrodes (e.g., graphite anode, <372 mAh g −1 ; LiCoO 2 cathode, <200 mAh g −1 ), [2] which have almost achieved the maximal energy density this system can deliver. In contrast, the lithium metal batteries (LMBs), employing high-capacity lithium metal as the anode (i.e., 3840 mAh g −1 ) and lithium layered metal oxide such as Nirich LiNi x Co y Mn z O 2 (NCM, x + y + z = 1) as cathode can realistically achieve a highenergy density (>400 Wh kg −1 ). [3] It is worth noting that the energy density can be further improved by enhancing the charge cut-off voltage to extract more lithium ions from the crystalline channels of the cathode. [4] For example, the Ni-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode can provide a capacity of more than 220 mAh g −1 when the cut-off voltage is equal to or higher than 4.3 V (versus Li/Li + ). [5] However, it is still a great challenge to design a stable electrolyte for high-voltage lithium metal batteries (LMBs).The electrolyte issues can be aggravated when high-Ni cathodes such as LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) are used since the reactive singlet oxygen ( 1 O 2 ) can be released at the highly delithiated states (>80%, i.e., the upper cut-off voltage is >4.2 V versus Li/Li + ), where these species can chemically oxidize the ethylene carbonate (EC) solvent in the High-voltage lithium metal batteries are the most promising energy storage technology due to their excellent energy density (>400 Wh kg −1 ). However, the oxidation decomposition of conventional carbonate-based electrolytes at the high-potential cathode, the detrimental reaction between the lithium anode and electrolyte, particularly the uncontrolled lithium dendrite growth, always lead to a severe capacity decay and/or flammable safety issues, hindering their practical applications. Herein, a solvation structure engineering strategy based on tuning intermolecular interactions is proposed as a strategy to design a novel nonflammable fluorinated electrolyte. Using this approach, this work shows superior cycling stability in a wide temperature range (−40 °C to 60 °C) for a 4.4 V-class LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)-based Li-metal battery. By coupling the high-loading of NCM811 cathode (3.0 mAh cm −2 ) and a controlled amount of lithium anode (twofold excess of Li deposition on Cu, Cu@Li) (N/P = 2), the Cu@Li || NCM811 full cell can cycle more than 162 cycles with high-capacity retention of 80%. This work finds that the change of the coordination environment of Li + with solvent and PF 6− by tuning intermolecular interaction is an effective method to stabilize the electrolyte and electrode performance. These discoveries can provide a pathway for electrolyte design in metal ion batteries.

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“…Therefore, F-containing cyclic carbonates represented by FEC are often used as co-solvents and additives, which have attracted wide attention in recent years. [29][30][31][32] Compared with the solvent containing the F atom, the anion is more effective at forming inorganic-rich films. Therefore, it has to be questioned whether the coordination between the anion and Li + will also promote the decomposition of the anion.…”

Section: Discovery Of the Anion-solvation Complex Regulating Eei Film...mentioning

confidence: 99%

Improving performances of the electrode/electrolyte interfaceviathe regulation of solvation complexes: a review and prospect

Yin

Yang

et al. 2023

Nanoscale

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Non‐Flammable Electrolyte Enables High‐Voltage and Wide‐Temperature Lithium‐Ion Batteries with Fast Charging

Cited by 96 publications

References 59 publications

Weak Solvent–Solvent Interaction Enables High Stability of Battery Electrolyte

Weak Solvent–Solvent Interaction Enables High Stability of Battery Electrolyte

Intermolecular Interactions Mediated Nonflammable Electrolyte for High‐Voltage Lithium Metal Batteries in Wide Temperature

Improving performances of the electrode/electrolyte interfaceviathe regulation of solvation complexes: a review and prospect

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