A Robust Li-Intercalated Interlayer with Strong Electron Withdrawing Ability Enables Durable and High-Rate Li Metal Anode

Chen, Jiahe; Li, Zhendong; Sun, Nannan; Xu, Jizheng; Li, Qian; Yao, Xiayin; Ming, Jun; Peng, Zhé

doi:10.1021/acsenergylett.2c00395

Cited by 48 publications

(23 citation statements)

References 36 publications

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“…[4][5][6][7] Without a sufficiently protective solidelectrolyte interphase (SEI) on LMAs, side reactions between lithium and electrolytes cause lithium dendritic growth and low stripping/plating coulombic efficiency (CE). [8][9][10] At the cathode/electrolyte interface, parasitic electrolyte degradation occurs due to the highly reactive Ni 4+ species generated upon delithiation. This is accelerated by increasing Ni content in the cathode, resulting in limited reversibility of the Ni-rich NMC cathode and thickening of the cathode/electrolyte interphase (CEI) upon cycling.…”

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confidence: 99%

Difluorobenzene‐Based Locally Concentrated Ionic Liquid Electrolyte Enabling Stable Cycling of Lithium Metal Batteries with Nickel‐Rich Cathode

Liu

Mariani

Diemant

et al. 2022

Advanced Energy Materials

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the high reactivity of both the lithium metal anode (LMA) and Ni-rich NMC usually leads to poor interfacial compatibility with the conventional electrolytes and consequently limited cyclability. [4][5][6][7] Without a sufficiently protective solidelectrolyte interphase (SEI) on LMAs, side reactions between lithium and electrolytes cause lithium dendritic growth and low stripping/plating coulombic efficiency (CE). [8][9][10] At the cathode/electrolyte interface, parasitic electrolyte degradation occurs due to the highly reactive Ni 4+ species generated upon delithiation. This is accelerated by increasing Ni content in the cathode, resulting in limited reversibility of the Ni-rich NMC cathode and thickening of the cathode/electrolyte interphase (CEI) upon cycling. [11,12] Among the strategies proposed to enhance the cyclability of LMBs, electrolyte engineering appears to be one of the most effective and feasible approaches, as the electrolyte plays a keyrole in the CEI and SEI formation. [13][14][15][16][17][18][19] Ionic liquid electrolytes (ILEs), with high electrochemical stability, are valuable options for Li/Ni-rich NMC cells in this context. [20][21][22][23] For instance, Wu et al. [24] have recently reported highly stable cycling of Li/LiNi 0.88 Co 0.09 Mn 0.03 O 2 cells up to 300 cycles with a capacity retention of 88% in [LiTFSI] 0.2 [Pyr 14 FSI] 0.8 (LiTFSI = lithium bis(trifluoromethanesulfonyl)imide, Pyr 14 FSI = N-butyl-Nmethyl pyrrolidinium bis(fluorosulfonyl)imide). Unfortunately, the excellent performance has been only achieved with low cathode mass loading (<5 mg cm −2 ), or/and low current density Lithium metal batteries (LMBs) with nickel-rich cathodes are promising candidates for next-generation, high-energy batteries. However, the highly reactive electrodes usually exhibit poor interfacial compatibility with conventional electrolytes, leading to limited cyclability. Herein, a locally concentrated ionic liquid electrolyte (LCILE) consisting of lithium bis(fluorosulfonyl)imide (LiFSI), 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide (EmimFSI), and 1,2-difluorobenzene (dFBn) is designed to overcome this challenge. As a cosolvent, dFBn not only promotes the Li + transport with respect to the electrolyte based on the ionic liquid only, but also has beneficial effects on the electrode/electrolyte interphases (EEIs) on lithium metal anodes (LMAs) and LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes. As a result, the developed LCILE enables dendritefree cycling of LMAs with a coulombic efficiency (CE) up to 99.57% at 0.5 mA cm −2 and highly stable cycling of Li/NMC811 cells (4.4 V) at C/3 charge and 1 C discharge (1 C = 2 mA cm −2 ) for 500 cycles with a capacity retention of 93%. In contrast, the dFBn-free electrolyte achieves lithium stripping/plating CE, and the Li/NMC811 cells' capacity retention of only 98.22% and 16%, respectively under the same conditions. The insight into the coordination structure, promoted Li + transport, and EEI characteristics gives fundamental information essential for fu...

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mentioning

confidence: 99%

Difluorobenzene‐Based Locally Concentrated Ionic Liquid Electrolyte Enabling Stable Cycling of Lithium Metal Batteries with Nickel‐Rich Cathode

Liu

Mariani

Diemant

et al. 2022

Advanced Energy Materials

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“…It also affects other physical properties of an electrolyte such as flammability, resisting overcharging, and ionic mobility at low temperatures, which would impact practical applications of the batteries. Aside from understanding the SEI effect, the comprehensive studies of the solvation structure and interfacial model (de)solvation process can guide the functional electrolyte design more effectively to improve the performance of ammonium-ion batteries, particularly with respect to high voltage, fast charge, and operation over an extended temperature range. − Spectroscopic analysis and theoretical simulations have been integrated to explore the intercalation mechanism of ammonium ions in the COFs above, confirming hydrogen bonds between NH 4 + ion and the COFs. Additionally, the solvation behaviors of Li + , Na + , K + , and NH 4 + ions were explored and compared, as displayed in Figure a–d, respectively.…”

Section: Electrode Materials For Ammonium-ion Batteriesmentioning

confidence: 99%

Recent Progress in Aqueous Ammonium-Ion Batteries

Wang

Kuchena

2022

ACS Omega

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Batteries using a water-based electrolyte have the potential to be safer, more durable, less prone to thermal runaways, and less costly than current lithium batteries using an organic solvent. Among the possible aqueous battery options, ammonium-ion batteries (AIBs) are very appealing because the base materials are light, safe, inexpensive, and widely available. This review gives a concise and useful survey of recent progress on emerging AIBs, starting with a brief overview of AIBs, followed by cathode materials, anode materials, electrolytes, and various devices based on ammonium-ion storage. Aside from summarizing the most updated electrodes/electrolytes in AIBs, this review highlights fundamental mechanistic studies in AIBs and state-of-the art applications of ammonium-ion storage. The present work reviews various theoretical efforts and the spectrum studies that have been used to explore ionic transport kinetics, electrolyte structure, solvation behavior of ammonium ions, and the intercalation mechanism in the host structure. Furthermore, diverse applications of ammonium-ion storage apart from aqueous AIBs are discussed, including flexible AIBs, AIBs that can operate across a wide temperature range, ammonium-ion supercapacitors, and battery–supercapacitor hybrid devices. Finally, the review is concluded with perspectives of AIBs, challenges remaining in the field, and possible research directions to address these challenges to boost the performance of AIBs for real-world practical applications.

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“…Copyright 2022 Wiley-VCH. (d) The electron withdrawing effect of intercalative anodes, as opposed to alloying or conversion-type anodes, to suppress electrolyte decomposition, reproduced from ref with permission. Copyright 2022 American Chemical Society.…”

Section: Anionic Activity In Bulk Phase Engineeringmentioning

confidence: 99%

“…In contrast to pure alloying/conversion-type anodes, which have a defect-rich surface during discharge that facilitates the electrolyte decomposition, the integrated electrodes with intercalative frameworks may have a significant electron withdrawing ability to suppress electrolyte decomposition even in the initial first cycle (Figure d), which benefits the improved cycling stability and high initial Coulombic efficiency.…”

Section: Anionic Activity In Bulk Phase Engineeringmentioning

confidence: 99%

Anionic Activity in Fast-Charging Batteries: Recent Advances, Prospects, and Challenges

Peng

Pang

et al. 2022

ACS Materials Lett.

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The increasing demand for fast-charging batteries to expedite the widespread adoption of electric vehicles calls for continual improvements of the anode materials to confer high energy and power densities. However, the fundamental limitations of the mainstream graphite and Li-metal anodes for fast-charging applications include the capacity fading and safety issues mainly caused by the Li plating, as well as the sluggish transport kinetics at large current densities. Recently, great attention has been paid to the emergence of large-capacity anodes by tailoring the bonding covalency to modulate the electronic structure and alter the insertion voltage for boosting fast-charging ability and suppressing metal plating. Development of new fast-charging materials by tailoring anionic activity allows us to better understand the key aspects of the bond covalency and band positioning for cation/anion doping and interface/ surface engineering. This Review provides an overview of the recent advances in the development of fast-charging anodes around tuning the bonding covalency by bimetal modulation; alloying hard and soft anions to alter the electronic structure and metal plating voltage; constructing anion-derived interfacial films; and surface substituting the ordered terminal groups. Furthermore, we highlight the practical limits of capacity fading at large current densities and describe potential strategies of anionic redox in phosphides and interfacial energy storage of conversion-type anodes to offer additional capacities. We also discuss the prospects for the commercial adoption of high-performance anodes containing various elements to rival the prevalent graphite or Li anodes for fast-charging applications.

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A Robust Li-Intercalated Interlayer with Strong Electron Withdrawing Ability Enables Durable and High-Rate Li Metal Anode

Cited by 48 publications

References 36 publications

Difluorobenzene‐Based Locally Concentrated Ionic Liquid Electrolyte Enabling Stable Cycling of Lithium Metal Batteries with Nickel‐Rich Cathode

Difluorobenzene‐Based Locally Concentrated Ionic Liquid Electrolyte Enabling Stable Cycling of Lithium Metal Batteries with Nickel‐Rich Cathode

Recent Progress in Aqueous Ammonium-Ion Batteries

Anionic Activity in Fast-Charging Batteries: Recent Advances, Prospects, and Challenges

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