A High‐Performance Carbonate‐Free Lithium|Garnet Interface Enabled by a Trace Amount of Sodium

Fu, Xingjie; Wang, Tiantian; Shen, Wenzhong; Jiang, Miaoli; Wang, Youwei; Dai, Qiushi; Wang, Da; Qiu, Zhenping; Zhang, Yelong; Deng, Kuirong; Zeng, Qingguang; Zhao, Ning; Guo, Xiangxin; Liu, Zheng; Liu, Jianjun; Peng, Zhangquan

doi:10.1002/adma.202000575

Cited by 71 publications

(52 citation statements)

References 28 publications

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“…The more intriguing results were observed in the "Li-Na" alloy case, which were published separately by Fu et al and Zhang et al at about the same time (Figure 7 (C,D)). 115,116 In both studies, it was observed that the addition of Na metal into molten Li depressed the contact angle and the interface ASR substantially. Nonetheless, the microstructures of the Li-Na molten mixtures are quite different because of the level of Na added.…”

Section: Intermetallic Interphases In Ssbsmentioning

confidence: 93%

Intermetallic interphases in lithium metal and lithium ion batteries

Sun

Peng

2021

InfoMat

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A robust electrode-electrolyte interface is the cornerstone for every battery system, as demonstrated in the meandering history of the development of Li-ion batteries (LIBs). In the thrust to replace the graphite anode with more energetic ones in LIBs, the effectual strategy for stabilizing the original graphiteelectrolyte interface becomes obsolete and a new anode-electrolyte interface needs reconfiguration. Unfortunately, this interface has become the Achilles' heel for those anodes, such as Li-metal anode (LMA) and Si-based anode owing to their excessive reductivity, enormous volume change, and so forth. Encouragingly, in the last decade, impressive progress has been made on taming these extremely unstable interfaces and on the solid-state batteries (SSBs) that are reported to be less susceptible to parasitic reactions. One of the distinguished strategies is the application of artificial Li-alloying intermetallic interphases onto the surface of LMA, via the direct introduction of foreign metals to the Li anode or indirect hetero-cations doping in the electrolyte, to regulate the Li deposition/ stripping behavior, which has markedly improved the stability of the LMAelectrolyte interface. In parallel, the intermetallic interphases are also witnessed to profoundly enhance the anode-solid electrolyte contact and the corresponding charge transfer kinetics in various SSBs. This review will provide a panoramic overview of the application of the intermetallic interphases at the anode-electrolyte interfaces in the lithium metal batteries (LMBs), SSBs, and also derivative works in the conventional LIBs, which will focus on different concepts, methodologies, and understandings from the encircled studies.

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Section: Intermetallic Interphases In Ssbsmentioning

confidence: 93%

Intermetallic interphases in lithium metal and lithium ion batteries

Sun

Peng

2021

InfoMat

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“…Most of the garnet‐typed electrolytes are unstable in moisture, forming Li‐ion insulating hydroxides and carbonates (such as Li 2 CO 3 ) on their surfaces, thereby increasing the interfacial resistance 90 . Therefore, Li 2 CO 3 prevention and removal is the key point to improve the interface properties between garnet‐typed SSEs with electrodes.…”

Section: Methods To Solve Interfacial Problemsmentioning

confidence: 99%

“…carbonates (such as Li 2 CO 3 ) on their surfaces, thereby increasing the interfacial resistance. 90 Therefore, Li 2 CO 3 prevention and removal is the key point to improve the interface properties between garnet-typed SSEs with electrodes. By controlling the grain size of LLZO particles, the surface sensitivity towards moisture and CO 2 can be optimized.…”

Section: Garnet/cathode Interfacementioning

confidence: 99%

Progress and perspective of interface design in garnet electrolyte‐based all‐solid‐state batteries

et al. 2021

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Inorganic solid-state electrolytes (SSEs) are nonflammable alternatives to the commercial liquid-phase electrolytes. This enables the use of lithium (Li) metal as an anode, providing high-energy density and improved stability by avoiding unwanted liquid-phase chemical reactions. Among the different types of SSEs, the garnet-type electrolytes witness a rapid development and are considered as one of the top candidates to pair with Li metal due to their high ionic conductivity, thermal, and electrochemical stability. However, the large resistances at the interface between garnet-type electrolytes and cathode/anode are the major bottlenecks for delivering desirable electrochemical performances of all-solid-state batteries (SSBs). The electrolyte/anode interface also suffers from metallic dendrite formation, leading to rapid performance degradation. This is a fundamental material challenge due to the poor contact and wettability between garnet-type electrolytes with electrode materials. Here, we summarize and analyze the recent contributions in mitigating such materials challenges at the interface. Strategies used to address these challenges are divided into different categories with regard to their working principles. On one hand, progress has been made in the anode/ garnet interface, such as the successful application of Li-alloy anode and different artificial interlayers, significantly improving interfacial performance. On the other hand, the desired cathode/garnet interface is still hard to reach due to the complex chemical and physical structure at the cathode. The common methods used are nanostructured cathode host and sintering additives for increasing the contact area.On the basis of this information, we present our views on the remaining challenges and future research of electrode/garnet interface. This review not only motivates the need for further understanding of the fundamentals, stability, and modifications of the garnet/electrode interfaces but also provides guidelines for the future design of the interface for SSB.

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“…The LLZTO pellets (12 mm in diameter, 1 mm in thickness) and LLZTO particles ( D 50 = 200–400 nm) were synthesized via solid-state reactions as reported previously . The obtained LLZTO ceramics have a relative density of 99.6%.…”

Section: Methodsmentioning

confidence: 99%

“…Solid-state lithium-metal batteries (SSLMBs) have drawn broad attention owing to their potential high energy densities and improved safety. Solid-state electrolytes (SSEs) play critical roles in the performance of SSLMBs. , Among all of the SSEs, garnet-type oxide (e.g., Li 7 La 3 Zr 2 O 12 , LLZO) or its derivatives (e.g., Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 , LLZTO) is a promising candidate owing to its high Li + conductivity at 25 °C, , wide electrochemical stability window and high chemical stability against Li anode. , Despite these merits, the development of LLZO-based SSLMBs is hampered by poor physical contact at the electrode/SSE interface, heterogeneous deposition of Li, and growth of Li dendrites from the anode. − Numerous strategies such as Li-alloy electrodes, − interlayers between Li and SSEs, − Li hosts in the anode, − lithiated graphite, and Li-metal ink are explored to reduce Li nucleation barrier through changing the lithiophobic Li/SSE interface to lithiophilic one. , Among the strategies based on Li-alloy electrodes, most alloy electrodes such as LiAl, , LiIn, LiSn, , and LiSi , suffer from pulverization due to alloying/dealloying reactions between Li and Al, In, Sn, and Si, thus limiting the cycle lifetime of LMBs. Recently, there are several reports of using metal such as Cu, which is chemically inert with Li, to be the Li host.…”

Section: Introductionmentioning

confidence: 99%

Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCu_x Nanowire Network Host

Dai

Zhao

et al. 2021

ACS Appl. Mater. Interfaces

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High interfacial resistance and uncontrollable lithium (Li) dendrite are major challenges in solid-state Li-metal batteries (SSLMBs), as they lead to premature short-circuiting and failure of SSLMBs. Here, we report the synthesis of a composite anode comprising a three-dimensional LiCu x nanowire network host infiltrated with Li (Li* anode) with low interfacial impedance and superior electrochemical performance. The Li* anode is fabricated by dissolving Cu foil into molten Li followed by solidification. The Li* anode exhibits good wettability with Li6.4La3Zr1.4Ta0.6O12 (LLZTO) and high mechanical strength, rendering low Li*/LLZTO interfacial impedance, homogeneous deposition of Li, and suppression of Li dendrites. Consequently, the Li* anode-based symmetric cells and full cells with LiNi0.88Co0.1Al0.02O2 (NCA), LiFePO4 (LFP), and FeF2 cathodes deliver remarkable electrochemical performance. Specifically, the Li*/LLZTO/Li* symmetrical cell achieves a remarkably long cycle lifetime of 10 000 h with 0.1 mA·cm–2; the Li*/LLZTO/NCA full cell maintains capacity retention of 73.4% after 500 cycles at 0.5C; and all-solid-state Li*/LLZTO/FeF2 full cell achieves a reversible capacity of 147 mAh·g–1 after 500 cycles at 100 mA·g–1. This work demonstrates potential design tactics for an ultrastable Li*/garnet interface to enable high-performance SSLMBs.

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A High‐Performance Carbonate‐Free Lithium|Garnet Interface Enabled by a Trace Amount of Sodium

Cited by 71 publications

References 28 publications

Intermetallic interphases in lithium metal and lithium ion batteries

Intermetallic interphases in lithium metal and lithium ion batteries

Progress and perspective of interface design in garnet electrolyte‐based all‐solid‐state batteries

Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCu_x Nanowire Network Host

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A High‐Performance Carbonate‐Free Lithium|Garnet Interface Enabled by a Trace Amount of Sodium

Cited by 71 publications

References 28 publications

Intermetallic interphases in lithium metal and lithium ion batteries

Intermetallic interphases in lithium metal and lithium ion batteries

Progress and perspective of interface design in garnet electrolyte‐based all‐solid‐state batteries

Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCux Nanowire Network Host

Contact Info

Product

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Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCu_x Nanowire Network Host