Achieving high capacity in bulk-type solid-state lithium ion battery based on Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 electrolyte: Interfacial resistance

Liu, Ting; Ren, Yaoyu; Shen, Yang; Zhao, Shunzheng; Lin, Yuan‐Hua; Nan, Ce‐Wen

doi:10.1016/j.jpowsour.2016.05.111

Cited by 154 publications

(94 citation statements)

References 25 publications

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“…Firstly, the Li-rich interphase was formed through Li migration from Li metal into garnet inner surface and from deeper garnet bulk to inner surface, the above Li-rich interphase and the Li wettability to garnet has been confirmed experimentally and theoretically. [25][26][27] Different Li 2 CO 3 formation mechanisms have been recently investigated and proposed, including direct reaction with products of ZrO 2 and La 2 O 3 , [28] reaction mediated by preliminary Li-H exchange, [29][30][31] or reaction mediated by defects as Li/O vacancies. These above two steps concurrently determine the theoretical overall ASR, which was calculated as the magnitude order of which was calculated as 10 −2 ·cm 2 under ideal conditions.…”

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confidence: 99%

The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li₇La₃Zr₂O₁₂ Interphase

Gao

Guo

Li³

et al. 2019

Advcd Theory and Sims

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The solid-solid interfacial impedance between the garnet electrolyte and Li metal anode is one of the major challenges for garnet's application in all-solid-state batteries. The areal specific resistance (ASR) is investigated by ab initio calculations in this article, to predict the intrinsic ASR as lower limitation. The Li ion migration across the interphase is divided into two steps: 1) Li "intercalation" from Li-metal to the LLZO, forming a Li-rich interphase beneath the surface of LLZO, and 2) Li migration in the Li-rich interphase within LLZO. The first step is investigated by climbing image nudged elastic band (CI-NEB), resulting in barrier energy lower than 0.37 eV compared to experimental 0.34 eV of the garnet bulk phase. The second step is investigated by ab initio molecular dynamic simulations (AIMD), indicating that the Li-rich interphase's conductivity is lower by about 1-2 orders of magnitude compared to the bulk phase. As a result, the sum theoretical intrinsic ASR is as low as 0.01 cm 2 , suggesting high ASR in practicable battery arises from surficial impurity Li 2 CO 3 rather than intrinsic ionic resistance. However, difficulties of removing Li 2 CO 3 lie in that Li 7 La 3 Zr 2 O 12 can thermodynamically decompose into reactive Li 2 O to form high resistant Li 2 CO 3 .With the rapid application and promotion of lithium ionbased electric or hybrid electric vehicles, the demand on safety and energy density is becoming more and more critical. As the flammable organic liquid electrolyte is the main case of the urgent safety problem, the solid electrolytes (SEs) without flammable organic small molecular liquid gradually attracts wide attention, including inorganic ceramic electrolytes and dry organic polymer electrolytes. [1] On the other hand, since the energy density upgrade of cathode could not fully meet the requirements, Li metal anode with a high capacity of 3860 mAh g −1 (about 1 order of magnitude higher than its graphite counterpart of 372 mAh g −1 ) is revived as a silver bullet for the demanding energy density. However, the lithium metal anode shows poor compatibility with traditional organic liquid electrolyte owing to a continuously evolving Li/electrolyte interface during charge/discharge. This insurmountable hurdle becomes soluble with suitable SEs, since a long-term stable interface of Li/SE is more accessible with the help of nonflowable solid electrolyte. Requirements on SEs include higher conductivity than 10 −4 S cm −1 at room temperature as the threshold for running a regular cell, [2] negligible electronic conductivity, wide electrochemical stability window, and high chemical and electrochemical stability with electrodes. Among the existing SEs including Li 3 N, [3] Na superionic conductor (NASICON), [4] perovskite, garnet, thio-γ -Li 3 PO 4 related system [5] (including glass and glass-ceramic states), thio-Li superionic conductor (LISICON), [6] and Li 10 GeP 2 S 12 , [7] garnet structured Li ionic conductors attract dominated interests in recent years [8,9] mainly owing to an a...

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confidence: 99%

The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li₇La₃Zr₂O₁₂ Interphase

Gao

Guo

Li³

et al. 2019

Advcd Theory and Sims

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“…[30] Thin-film batteries have a low energy density and a long lead time due to the deposition of the electrolyte and electrode materials, which has limited their wide application, such as in power batteries in electric vehicles. [31] Therefore, recent studies have focused on the application of OCEs to improve the energy density, power density and production efficiency of ASSLBs. [31][32][33] ASSLBs based on OCEs have a distinct difference in internal Li + transmission dynamics compared to liquid LIBs.…”

Section: Introductionmentioning

confidence: 99%

“…[31] Therefore, recent studies have focused on the application of OCEs to improve the energy density, power density and production efficiency of ASSLBs. [31][32][33] ASSLBs based on OCEs have a distinct difference in internal Li + transmission dynamics compared to liquid LIBs. OCEs have shown a Li + conductivity of up to 10 À 3 S cm À 1 , which gradually approaches liquid electrolytes (10 À 2 S cm À 1 ).…”

Section: Introductionmentioning

confidence: 99%

Reducing the Interfacial Resistance in All‐Solid‐State Lithium Batteries Based on Oxide Ceramic Electrolytes

2019

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All‐solid‐state lithium batteries (ASSLBs) are regarded as next‐generation advanced energy‐storage devices, owing to their high energy density and safety. The interfacial resistance is a crucial factor affecting the practical application of ASSLBs. ASSLBs based on oxide‐based ceramic electrolytes (OCEs) still exhibit poor electrochemical performance, owing to the large interfacial resistance. Area‐specific resistance values at the interfaces ranging from thousands of ohms to several ohms per square centimeter have been achieved using multiple strategies. This Review summarizes multiple existing advanced strategies used to reduce the interfacial resistance between OCEs and electrodes through interfacial engineering. We also propose some perspectives for the future development of ASSLBs based on OCEs.

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“…[1][2][3][4][5][6] However,the penetration of Li dendrites through the separator in batteries,w hich raises safety concerns and often results in battery performance decay,h ave limited the use of Li metal anodes for decades.R ecently,e xtensive studies of Li metal composites and modified separators to suppress or delay Li dendrite growth have been reported. [11,15,17,22,[34][35][36][37][38][39][40][41][42][43][44][45] Our recent progress has significantly decreased the garnet solid electrolyte/Li interface resistance by applying at hin metal interlayer,s uch as Al, Si, and Ge. [20,21,23] Among the different types of solid-state electrolytes,t he Li 7 La 3 Zr 2 O 12 (LLZO) garnet-type solid-state electrolyte is al eading candidate for Li metal batteries,due to its high ionic conductivity (10 À3 -10 À4 Scm) and chemical stability against Li metal.…”

mentioning

confidence: 99%

“…[20,21,23] Among the different types of solid-state electrolytes,t he Li 7 La 3 Zr 2 O 12 (LLZO) garnet-type solid-state electrolyte is al eading candidate for Li metal batteries,due to its high ionic conductivity (10 À3 -10 À4 Scm) and chemical stability against Li metal. [11,15,17,22,[34][35][36][37][38][39][40][41][42][43][44][45] Our recent progress has significantly decreased the garnet solid electrolyte/Li interface resistance by applying at hin metal interlayer,s uch as Al, Si, and Ge. [11,15,17,22,[34][35][36][37][38][39][40][41][42][43][44][45] Our recent progress has significantly decreased the garnet solid electrolyte/Li interface resistance by applying at hin metal interlayer,s uch as Al, Si, and Ge.…”

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confidence: 99%

Transient Behavior of the Metal Interface in Lithium Metal–Garnet Batteries

Gong

et al. 2017

Angewandte Chemie

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The interface between solid electrolytes and Li metal is aprimary issue for solid-state batteries.Introducing ametal interlayer to conformally coat solid electrolytes can improve the interface wettability of Li metal and reduce the interfacial resistance,b ut the mechanism of the metal interlayer is unknown. In this work, we used magnesium (Mg) as am odel to investigate the effect of am etal coating on the interfacial resistance of asolid electrolyte and Li metal anode.The Li-Mg alloyh as low overpotential, leading to al ower interfacial resistance.O ur motivation is to understand howt he metal interlayer behaves at the interface to promote increased Limetal wettability of the solid electrolyte surface and reduce interfacial resistance.S urprisingly,w ef ound that the metal coating dissolved in the molten piece of Li and diffused into the bulk Li metal, leading to as mall and stable interfacial resistance between the garnet solid electrolyte and the Li metal. We also found that the interfacial resistance did not change with increase in the thickness of the metal coating (5, 10, and 100 nm), due to the transient behavior of the metal interface layer.The adoption of lithium (Li)m etal as anode is critical to achieving high energy and high power density batteries since Li metal has the highest theoretical capacity (3860 mAh g À1 ) while maintaining the lowest electrochemical potential (À3.04 Vv ersus the standard hydrogen electrode). [1][2][3][4][5][6] However,the penetration of Li dendrites through the separator in batteries,w hich raises safety concerns and often results in battery performance decay,h ave limited the use of Li metal anodes for decades.R ecently,e xtensive studies of Li metal composites and modified separators to suppress or delay Li dendrite growth have been reported. [7][8][9][10][11][12][13][14] In comparison to those efforts,a na ll-in-one strategy is to use as olid-state electrolyte to replace polymer separators and physically block the Li dendrite penetration [15][16][17][18][19][20][21][22] Theu se of as olid-state electrolyte has many advantages over organic liquid electrolyte in batteries;f or example,as olid-state electrolyte generally has aw ide stability window (0-5 V), good thermal stability,a nd an intrinsic nonflammability. [20,21,23] Among the different types of solid-state electrolytes,t he Li 7 La 3 Zr 2 O 12 (LLZO) garnet-type solid-state electrolyte is al eading candidate for Li metal batteries,due to its high ionic conductivity (10 À3 -10 À4 Scm) and chemical stability against Li metal. [20,[23][24][25][26][27][28][29][30][31][32][33] Amajor challenge of using the garnet solid-state electrolyte in aL im etal battery is the poor contact at the interface between the garnet and the Li metal, leading to ah igh interfacial impedance of 10 2 -10 3 ohm cm À2 .E xtensive work has been reported to reduce the interfacial impedance,f or example,b ym odifying solid electrolyte composition, using gel or polymer interlayers,a nd constructing interface structures. [11,15,17,22,[34][35][36][37...

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Achieving high capacity in bulk-type solid-state lithium ion battery based on Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 electrolyte: Interfacial resistance

Cited by 154 publications

References 25 publications

The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li₇La₃Zr₂O₁₂ Interphase

The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li₇La₃Zr₂O₁₂ Interphase

Reducing the Interfacial Resistance in All‐Solid‐State Lithium Batteries Based on Oxide Ceramic Electrolytes

Transient Behavior of the Metal Interface in Lithium Metal–Garnet Batteries

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Achieving high capacity in bulk-type solid-state lithium ion battery based on Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 electrolyte: Interfacial resistance

Cited by 154 publications

References 25 publications

The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li7La3Zr2O12 Interphase

The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li7La3Zr2O12 Interphase

Reducing the Interfacial Resistance in All‐Solid‐State Lithium Batteries Based on Oxide Ceramic Electrolytes

Transient Behavior of the Metal Interface in Lithium Metal–Garnet Batteries

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The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li₇La₃Zr₂O₁₂ Interphase

The Ab Initio Calculations on the Areal Specific Resistance of Li‐Metal/Li₇La₃Zr₂O₁₂ Interphase