Building an Interfacial Framework: Li/Garnet Interface Stabilization through a Cu<sub>6</sub>Sn<sub>5</sub> Layer

Feng, Wuliang; Dong, Xiaoli; Lai, Zhengzhe; Zhang, Xinyue; Wang, Yonggang; Wang, Congxiao; Luo, Jiayan; Xia, Yongyao

doi:10.1021/acsenergylett.9b01158

Cited by 80 publications

(65 citation statements)

References 29 publications

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“… a Galvanostatic cycling performance of the Li/LLZTO/Li and Li/LLZTO@EBS/Li cells at 0.2 mA cm −2 (0.1 mAh cm −2 ) at 25 °C; b Magnified images for 0–20 h. c Galvanostatic cycling performance of the Li/LLZTO/Li and Li/LLZTO@EBS/Li cells at 0.5 mA cm −2 (0.25 mAh cm −2 ) at 25 °C; d Magnified images for 0–20 h. e Galvanostatic cycling performance of the Li/LLZTO@EBS/Li cell at 1 mA cm −2 (1 mAh cm −2 ) at 25 °C. f Galvanostatic cycling performance in recent literature compared with our work 20 , 21 , 28 , 35 , 37 , 58 , 59 . …”

Section: Resultsmentioning

confidence: 81%

A flexible electron-blocking interfacial shield for dendrite-free solid lithium metal batteries

et al. 2021

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Solid-state batteries (SSBs) are considered to be the next-generation lithium-ion battery technology due to their enhanced energy density and safety. However, the high electronic conductivity of solid-state electrolytes (SSEs) leads to Li dendrite nucleation and proliferation. Uneven electric-field distribution resulting from poor interfacial contact can further promote dendritic deposition and lead to rapid short circuiting of SSBs. Herein, we propose a flexible electron-blocking interfacial shield (EBS) to protect garnet electrolytes from the electronic degradation. The EBS formed by an in-situ substitution reaction can not only increase lithiophilicity but also stabilize the Li volume change, maintaining the integrity of the interface during repeated cycling. Density functional theory calculations show a high electron-tunneling energy barrier from Li metal to the EBS, indicating an excellent capacity for electron-blocking. EBS protected cells exhibit an improved critical current density of 1.2 mA cm−2 and stable cycling for over 400 h at 1 mA cm−2 (1 mAh cm−2) at room temperature. These results demonstrate an effective strategy for the suppression of Li dendrites and present fresh insight into the rational design of the SSE and Li metal interface.

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Section: Resultsmentioning

confidence: 81%

A flexible electron-blocking interfacial shield for dendrite-free solid lithium metal batteries

et al. 2021

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“…The materials include Al 2 O 3 , [46] ZnO, [42] SnO 2 , [75] SnF 2 , [76] MoS 2 , [77] AgNO 3 , [78] Cu 3 N, [79] and Cu 6 Sn 5 . [80] They play a similar role in increasing the wettability, so here we take Al 2 O 3 as an example. Han with a higher binding energy of 6.0-11.4 eV nm -2 than that of 1.6 eV nm -2 for Li 2 CO 3 , increased the contact angle and decreased the interfacial resistance to 1 Ω cm 2 ( Figure 4I).…”

Section: Artificial Interlayermentioning

confidence: 99%

“…These vacancies formed in Li metal can either annihilate after repeatable growth or diffuse from the interface into the bulk. Because the charge transfer [80] resistance is quite small and the Li + mobility in bulk garnets is very high, vacancy diffusion in Li metal dominates the interfacial dynamics when vacancy annihilation is excluded for simplicity. 1) If the diffusion coefficient of vacancies in Li metal is high enough, a dynamic balanced vacancy concentration at the interface will be established and the interface will keep morphologically stable.…”

Section: LImentioning

confidence: 99%

Interfaces in Garnet‐Based All‐Solid‐State Lithium Batteries

Wang

Zhu

et al. 2020

Advanced Energy Materials

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liquid electrolytes. ASSLBs exhibit overwhelming advantages as follows: 1) No electrolyte leakage. The most obvious advantage of ASSLBs is the avoidance of electrolyte leakage, and related issues such as fire hazard, electrical short circuit and corruption. In addition, ASSLBs do not need advance sealants, pressurizing electrolyte, and flame retardant failsafe. [1,2] 2) No thermal runaway. Thermal runaway will cause the rise of internal temperature, pressure, and vent of flammable gases in conventional LIBs, at a risk of explosion and shrapnel. [3,4] ASSLBs avoid the use of organic electrolytes and prevent the thermal runaway for a large extent. [5] 3) High resistance to lithium dendrite. The lithium dendrite may form during deposition process and penetrate through the separator, potentially cause a short circuit in conventional LIBs. [6] ASSLBs using solid electrolytes (SEs) with high shear modulus are expected to prevent/alleviate the dendrite penetration and extend the cell life. 4) Higher energy density. [7] The conventional LIBs are not suitable for the application of high voltage cathode and lithium metal anode because of narrow electrochemical window of liquid electrolytes, as well as failure in preventing lithium dendrite. ASSLBs facilitate the application of high voltage cathode materials and high energy density lithium metal anode, therefore increasing the energy density of the whole cell. Figure 1 shows the scheme of a typical ASSLB. Similar with conventional LIBs, the main components of ASSLB are cathode, SE, and anode. The distinctive component is SE, and its properties support the great advantages of ASSLBs. These properties include stability at ultrahigh and ultralow temperature, high mechanical strength, [8] wider electrochemical window (with passivation), and so on. [9-11] According to the category of SE, ASSLBs are divided into polymer-based, oxide-based, and sulfide-based systems, corresponding to the polymer, oxide, and sulfide electrolytes, respectively. Therein, oxide electrolytes exhibit moderate ionic conductivity, high shear modulus, and better stability with atmosphere and electrodes, are promising candidates for ASSLB. Specifically, oxide electrolytes are classified into LISICON (Li 14 ZnGe 4 O 16), NASICION (LiTi 2 (PO 4) 3), perovskite (Li 3x La 0.67-x □ 0.33-2x TiO 3), garnet (Li 3-7 LnMO 12 , Ln = Y, Pr, Nd, La, Sm-Lu, M = Zr, Sb, W, etc.), and so on based on their structure. Without reductive Ge, Ti elements in the composition, garnets are normally considered most promising among oxide electrolytes. [12,13] Garnet-type electrolytes in the formula of Li 3-7 Ln 3 M 2 O 12 , show a space group 3 Ia d. Lithium content ranges from 3 to 7 based on the substitution elements at Ln and M sites. [14,15] All-solid-state lithium batteries (ASSLBs) are considered to be the nextgeneration energy storage system, because of their overwhelming advantages in energy density and safety compared to conventional lithium ion batteries. Among various systems, garnet-based ASSLBs are one of the most promis...

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“…[46] In response, Feng et al reported a Cu 6 Sn 5 alloy interlayer with limited Sn diffusion and stable framework that could effectively mitigate the volume change for maintaining a good interface contact. [47] Recently, adding ion conductors into alloy interlayers has been investigated to enable superior battery performance. [33] A new study from Sun's group designed a mixed conductive layer (MCL) by embedding electronic conductive Cu nanoparticles into Li 3 N ionic conductive network through reacting the Cu 3 N film with molten LM.…”

Section: Alloy Interlayersmentioning

confidence: 99%

Interface between Lithium Metal and Garnet Electrolyte: Recent Progress and Perspective

Wang

Huang

Zhang

2020

Batteries & Supercaps

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Garnet electrolytes (GEs) with high ion conductivity, excellent stability against lithium metal (LM) as well as wide electrochemical potential window are attracting increasing interest as they have the potential to enable all-solid-state Li metal batteries (ASSLMBs). However, GEs-based ASSLMBs deeply suffer from daunting problems such as high resistance, fast short circuit, and rapid performance degradation, which can be largely attributed to unsatisfactory LM/GE interface. To this end, this minireview focuses on the LM/GE interface by summarizing the main challenges comprehensively, recapitulating emerging strategies for these challenges, and providing perspectives for future research.

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Building an Interfacial Framework: Li/Garnet Interface Stabilization through a Cu₆Sn₅ Layer

Cited by 80 publications

References 29 publications

A flexible electron-blocking interfacial shield for dendrite-free solid lithium metal batteries

A flexible electron-blocking interfacial shield for dendrite-free solid lithium metal batteries

Interfaces in Garnet‐Based All‐Solid‐State Lithium Batteries

Interface between Lithium Metal and Garnet Electrolyte: Recent Progress and Perspective

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Building an Interfacial Framework: Li/Garnet Interface Stabilization through a Cu6Sn5 Layer

Cited by 80 publications

References 29 publications

A flexible electron-blocking interfacial shield for dendrite-free solid lithium metal batteries

A flexible electron-blocking interfacial shield for dendrite-free solid lithium metal batteries

Interfaces in Garnet‐Based All‐Solid‐State Lithium Batteries

Interface between Lithium Metal and Garnet Electrolyte: Recent Progress and Perspective

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Building an Interfacial Framework: Li/Garnet Interface Stabilization through a Cu₆Sn₅ Layer