Locally Saturated Ether-Based Electrolytes With Oxidative Stability For Li Metal Batteries Based on Li-Rich Cathodes

Holoubek, John; Liu, Haodong; Yan, Qizhang; Wu, Zhaohui; Qiu, Bao; Zhang, Minghao; Yu, Sicen; Wang, Shen; Zhou, Jianbin; Pascal, Tod A.; Luo, Jian; Liu, Zhaoping; Meng, Ying Shirley; Liu, Ping

doi:10.1021/acsami.3c07224

Cited by 6 publications

(3 citation statements)

References 39 publications

(73 reference statements)

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“…Many strategies are used to improve the capacity retention of the Ni-rich NMC cathode. One common strategy is to coat a Li-ion-based conductive layer, such as LiNbO 3, , Li 2 TiO 3 , , LiAlO 2 , , and Li 2 ZrO 3 . , The spontaneous reactions between the electrolyte and cathode are minimized via surface modification to improve the electrochemical stability. Coating inhibits transition-metal (TM) dissolution in the electrolyte and improves structural stability. , Another method is to synthesize NMC by creating a concentration gradient.…”

Section: Introductionmentioning

confidence: 99%

Artificial Layer Construction via Cosolvent Enables Stable Ni-Rich Cathodes for Enhanced Lithium Storage

Pan,

Liu,

Hou

2024

ACS Appl. Mater. Interfaces

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Ni-rich cathodes have recently gained significant attention as next-generation cathodes for lithium-ion batteries. However, their relatively high oxidative surface should be reduced to control the high surface reactivity because the capacity retention decreases rapidly in the batteries. Herein, a simple and effective method to pretreat LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) particles using a cosolvent for improving the battery performance is reported. Imitating the interfacial reaction in practical cells, an artificial layer is created via a spontaneous redox reaction between the cathode and the organic solvent. The artificial layer comprises metal− organic compounds with reduced transition-metal cations. Benefiting from the artificial layer, the cells deliver high capacity retention at a high current density and better rate capability, which might result from the low and stable interfacial resistance of the modified NMC811 cathode. Our approach can effectively reduce the high oxidative surface of most oxide cathode materials and induce a long cyclic lifespan and high capacity retention in most battery systems.

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Section: Introductionmentioning

confidence: 99%

Artificial Layer Construction via Cosolvent Enables Stable Ni-Rich Cathodes for Enhanced Lithium Storage

Pan,

Liu,

Hou

2024

ACS Appl. Mater. Interfaces

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“…30 However, those ester-based and ether-based LHCEs were primarily designed for commercial cathode materials, such as LiNi x Co y Mn z O 2 (x + y + z = 1, NCM), 31,32 with much less attention devoted to their compatibility with LRMO cathode materials. 33 Therefore, understandings of the interfacial stability of LHCEs on the LRMO cathode, especially the discrepancy between etherbased and ester-based LHCEs, and the design principle of LHCEs for the LRMO cathode remain limited.…”

Section: Introductionmentioning

confidence: 99%

“…Compared to commercial carbonate electrolytes, ester-based LHCEs exhibit better dendrite suppression on Li metal anode. , In addition, ether-based LHCEs exhibit superior oxidative stability compared with conventional dilute ether-based electrolytes . However, those ester-based and ether-based LHCEs were primarily designed for commercial cathode materials, such as LiNi x Co y Mn z O 2 ( x + y + z = 1, NCM), , with much less attention devoted to their compatibility with LRMO cathode materials . Therefore, understandings of the interfacial stability of LHCEs on the LRMO cathode, especially the discrepancy between ether-based and ester-based LHCEs, and the design principle of LHCEs for the LRMO cathode remain limited.…”

Section: Introductionmentioning

confidence: 99%

Comparative Study of Lithium-Rich Cathode in Ester- and Ether-Based Localized High-Concentration Electrolytes

Guo,

Li,

Jie

et al. 2024

Energy Fuels

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Lithium-rich manganese oxide (LRMO)-based lithium metal batteries (LRMO-LMBs) are prospective options for future electrochemical storage systems. The performance of the LRMO-LMBs is significantly influenced by the electrolyte. The comprehension of the correlation between electrolyte formulation and electrode stability is crucial in guiding the design of advanced electrolytes for enhancing cell performance. Herein, we systematically study the interfacial behavior of localized high-concentration electrolytes (LHCEs) and their effect on cathode stability in the Li||LRMO system, selecting typical LHCEs using 1,2-dimethoxyethane (DME) and dimethyl carbonate (DMC) solvents. On the LRMO surface, DME-LHCE tends to undergo uncontrollable oxidation at 4.8 V, which leads to severe structural degradation of LRMO. Moreover, it causes increased dissolution of transition metal ions that subsequently deposit on the Li metal anode, thereby accelerating anode failure. Conversely, DMC-LHCE forms more stable electrode/electrolyte interphases, which effectively protect both the cathode and anode. Consequently, the Li||LRMO cell using DMC-LHCE shows excellent cycling performance, maintaining 96.6% capacity retention over 100 cycles at 0.5 C. This study offers insights into the compatibility between LHCEs and LRMO, facilitating electrolyte design for LRMO-LMBs.

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Understanding and Design of Cathode–Electrolyte Interphase in High‐Voltage Lithium–Metal Batteries

Li,

He,

Jie

et al. 2024

Adv Funct Materials

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The development of lithium–metal batteries (LMBs) has emerged as a mainstream approach for achieving high‐energy‐density energy storage devices. The stability of electrochemical interfaces plays an essential role in realizing stable and long‐life LMBs. Despite extensive and comprehensive research on the lithium anode interface, there is limited focus on the cathode interface, particularly regarding high‐voltage transition metal oxide cathode materials. In this review, the challenges associated with developing stable high‐voltage cathode materials are first discussed. Characterization techniques for understanding the composition and structure of the cathode–electrolyte interphase (CEI) are then introduced. Subsequently, recent developments in electrolyte design and interface modification for constructing a stable CEI are summarized. Finally, perspectives on future research trends for understanding and developing the high‐voltage CEI are discussed. This review can offer valuable guidance for understanding and designing the high‐voltage CEI, pushing forward the development of high‐energy‐density LMBs.

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Locally Saturated Ether-Based Electrolytes With Oxidative Stability For Li Metal Batteries Based on Li-Rich Cathodes

Cited by 6 publications

References 39 publications

Artificial Layer Construction via Cosolvent Enables Stable Ni-Rich Cathodes for Enhanced Lithium Storage

Artificial Layer Construction via Cosolvent Enables Stable Ni-Rich Cathodes for Enhanced Lithium Storage

Comparative Study of Lithium-Rich Cathode in Ester- and Ether-Based Localized High-Concentration Electrolytes

Understanding and Design of Cathode–Electrolyte Interphase in High‐Voltage Lithium–Metal Batteries

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