Dendrite-Free and Micron-Columnar Li Metal Deposited from LiNO<sub>3</sub>-Based Electrolytes

Zhou, Jingjing; Chen, Jiahang; Yang, Jun; Nuli, Yanna; Wang, Jiulin

doi:10.1021/acsaem.1c02158

Cited by 12 publications

(8 citation statements)

References 42 publications

(74 reference statements)

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“…After getting decomposed the N adsorbs at the surface interacting with Li and Al forming compounds like Li x Al y N (Figure 3a). The favourable decomposition of NO 3 over PF 6 could be the reason that in experimental reports Li 3 N is found to be a major component of the formed SEI layer [16,25,48] . The quicker diffusion of NO 3 towards the surface compared to that of PF 6 during the simulation could be another reason (Figure S2a).…”

Section: Resultsmentioning

confidence: 71%

“…[24] There are also reports of using LiNO 3 as additive in ether-based solvents, but they exhibit a lower electrochemical window. [16,25] On the other hand, this report showed that LiNO 3 with carbonate-based solvent can control uniform SEI deposition in a battery operating at higher voltage. [24] Lithium bis(fluorosulfonyl)imide (LiFSI) has also been used due to its ability to form a uniformly deposited SEI layer.…”

Section: Introductionmentioning

confidence: 85%

“…Recently, a LiNO 3 modified carbonate‐based electrolyte has been used in a LiPF 6 dual‐ion battery to mitigate the nonuniform Li nucleation/growth because of which longer cycle life and capacity retention could be achieved [24] . There are also reports of using LiNO 3 as additive in ether‐based solvents, but they exhibit a lower electrochemical window [16,25] . On the other hand, this report showed that LiNO 3 with carbonate‐based solvent can control uniform SEI deposition in a battery operating at higher voltage [24] .…”

Section: Introductionmentioning

confidence: 94%

“…The favourable decomposition of NO 3 over PF 6 could be the reason that in experimental reports Li 3 N is found to be a major component of the formed SEI layer. [16,25,48] The quicker diffusion of NO 3 towards the surface compared to that of PF 6 during the simulation could be another reason (Figure S2a). The LiAl surface is found to transfer 15.90 j e j charge to the electrolyte during simulation (Table S2).…”

Section: Lipf 6 and Linomentioning

confidence: 99%

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Lithium Nitrate as Salt Additive for Solid Electrolyte Interphase Formation in Dual‐Ion Battery

Pathak

Das

2023

Batteries & Supercaps

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Tuning the solid electrolyte interphase (SEI) formation in dual‐ion batteries is important for improving their long‐term stability. In this context, salt additives have gained importance which can sacrificially undergo reduction thereby protecting the working salt. Herein, we have considered dual salt electrolyte models of LiNO3 additive with LiPF6 and LiFSI salt to carry out ab initio molecular dynamics (AIMD) simulations and witness the evolution of SEI layer. Various contact ion pair and solvent separated ion pair models of the dual salt electrolytes have been considered to further understand the role played by solvation shells of the ions. The small size and quicker diffusion of anions through the electrolyte results in its decomposition at the electrode surface irrespective of the anion being in contact ion pair or solvated by solvent molecules. Overall, along with underlining the role of salt additives in SEI formation, this detailed study also provides insights regarding the factors beyond solvation characteristics of salt that determines the SEI growth process.

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Section: Resultsmentioning

confidence: 71%

Section: Introductionmentioning

confidence: 85%

Section: Introductionmentioning

confidence: 94%

Section: Lipf 6 and Linomentioning

confidence: 99%

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Lithium Nitrate as Salt Additive for Solid Electrolyte Interphase Formation in Dual‐Ion Battery

Pathak

Das

2023

Batteries & Supercaps

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“…A columnar Li deposition is thus desirable. [133,134] Suitable external pressure is also favorable to maintain close contact between the individual Li particles and drive the lean electrolyte to effectively wet the newly formed Li surfaces. [43] Li metal anode matching high voltage cathode is desirable to render a high-energy-density pouch cell.…”

Section: Regulating Electrolytesmentioning

confidence: 99%

Working Principles of Lithium Metal Anode in Pouch Cells

Sun

Cheng

et al. 2022

Advanced Energy Materials

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Advanced energy storage technology represented by lithium (Li)-ion batteries (LIBs) has revolutionized human life in recent years. The energy density of LIBs based on intercalation chemistry is approaching its theoretical limit after unremitting efforts for the past three decades. The state-of-the-art LIBs with graphite anode can only achieve an energy density lower than 300 Wh kg −1 . [1] This cannot satisfy the increasing demands for portable electronic devices, electric vehicles, and stationary energy storage systems. [2] Therefore, it is urgently called for next-generation batteries with a high energy density, long lifespan, and high safety performance. [3,4] Electrode material is of great importance in determining the energy density of batteries. [5] As the holy grail anode, Li metal possesses the ultrahigh theoretical specific capacity (3860 mAh g −1 ) and low potential (−3.04 V vs the standard hydrogen electrode). The promising feature renders Li metal anode to be an indispensable candidate for constructing next-generation high-energy-density batteries. [6] A high energy density of 400 or even 500 Wh kg −1 can be achieved with Li metal batteries (LMBs) matching Ni-rich LiNi x Co y Mn (1−x−y) O 2 (0 < x, y <1), oxygen, or sulfur cathodes, etc. [7][8][9] However, the conversion chemistry and high reactivity of Li metal also bring great challenges to the design of robust LMBs with long lifespan and high safety. [10,11] Specifically, Li dendrite growth and infinite volume variation lead to unstable solid electrolyte interphase (SEI) on Li metal anodes, resulting in low Li utilization, capacity decline, and even safety risk, [12] severely hindering the practical applications of LMBs. [13][14][15] Recently, extensive strategies have been exploited to control the dendrite growth of Li metal anodes, including engineering electrolytes and additives, [16] designing 3D host structures, [17][18][19] constructing artificial SEI, [20,21] applying solid-state electrolyte (SSE), [22][23][24] and adjusting operation conditions. [25] A high Coulombic efficiency (>99.9%) and long lifespan (>1000 cycles) have been reported in the materials-level coin cells. [26][27][28] Notably, Li dendrite growth is primarily driven by the kinetical limitation of Li-ion diffusion near the electrolyte/electrode interface. Serious dendrite issues can be encountered under harsh operating conditions in pouch cells, considering the accelerated consumption of Li ions at large currents and high Lithium metal battery has been considered as one of the potential candidates for next-generation energy storage systems. However, the dendrite growth issue in Li anodes results in low practical energy density, short lifespan, and poor safety performance. The strategies in suppressing Li dendrite growth are mostly conducted in materials-level coin cells, while their validity in device-level pouch cells is still under debate. It is imperative to address dendrite issues in pouch cells to realize the practical application of Li metal batteries. This review prese...

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Interphase‐Designable Additive‐Enabled Ethylene Carbonate‐Free Electrolyte for Wide‐Temperature, Long‐Cycling, High‐Voltage Lithium Metal Batteries

Huang,

Li,

Liu

et al. 2024

Adv Funct Materials

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Increasing the upper cut‐off voltage of the LiNixCoyMn1‐x‐yO2 (NCM)‐based lithium‐metal batteries (LMBs) is highly pursued for achieving high battery energy density. However, the cycling stability of high‐voltage LMBs, which is associated with ethylene carbonate electrolytes, remains greatly challenging. Herein, an interphase‐designable additive‐enabled ethylene carbonate‐free electrolyte strategy is proposed for achieving 4.6 V Li||NCM811 battery with long cycling life from 55 to −30 °C. The solvent characteristics of ethyl methyl carbonate endow LMBs with potential merits in high voltage, wide temperature, and cycling stability, which are further strengthened by the additive, 1,5‐difluoro‐2,4‐dinitrobenzene (FNB), for optimizing electrode electrolyte interphases. The sturdy LiF‐rich and LiNxOy‐contained electrode/electrolyte interphase on cathode/anode surfaces can protect two electrodes well from electrolyte corrosion and also reduce excessive electrolyte decomposition. As expected, the Li||NCM811 batteries can maintain 70% capacity retention after 500 cycles with superior high‐temperature and low‐temperature performance (from 55 to −30 °C). The 6.8Ah pouch cells with this electrolyte can achieve a high energy density of up to 505 Wh kg−1.

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Dendrite-Free and Micron-Columnar Li Metal Deposited from LiNO₃-Based Electrolytes

Cited by 12 publications

References 42 publications

Lithium Nitrate as Salt Additive for Solid Electrolyte Interphase Formation in Dual‐Ion Battery

Lithium Nitrate as Salt Additive for Solid Electrolyte Interphase Formation in Dual‐Ion Battery

Working Principles of Lithium Metal Anode in Pouch Cells

Interphase‐Designable Additive‐Enabled Ethylene Carbonate‐Free Electrolyte for Wide‐Temperature, Long‐Cycling, High‐Voltage Lithium Metal Batteries

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Dendrite-Free and Micron-Columnar Li Metal Deposited from LiNO3-Based Electrolytes

Cited by 12 publications

References 42 publications

Lithium Nitrate as Salt Additive for Solid Electrolyte Interphase Formation in Dual‐Ion Battery

Lithium Nitrate as Salt Additive for Solid Electrolyte Interphase Formation in Dual‐Ion Battery

Working Principles of Lithium Metal Anode in Pouch Cells

Interphase‐Designable Additive‐Enabled Ethylene Carbonate‐Free Electrolyte for Wide‐Temperature, Long‐Cycling, High‐Voltage Lithium Metal Batteries

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Dendrite-Free and Micron-Columnar Li Metal Deposited from LiNO₃-Based Electrolytes