Demonstration of high current densities and extended cycling in the garnet Li7La3Zr2O12 solid electrolyte

Taylor, Nathan J.; Stangeland-Molo, Sandra; Haslam, Catherine G.; Sharafi, Asma; Thompson, Travis; Wang, Michael J.; Garcia‐Mendez, Regina; Sakamoto, Jeff

doi:10.1016/j.jpowsour.2018.06.055

Cited by 147 publications

(120 citation statements)

References 23 publications

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“…So far, the most critical challenge is how to enhance the capability of suppressing dendrite penetration while maintaining a lower interfacial impedance between SSE and Li metal, particularly under the practical conditions of high current density (>1.0 mA cm −2 ). [ 9,10–12 ] Garnet‐type solid electrolytes (GSEs), such as Ta‐doped Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO), are regarded as the ideal SSEs, because of their high Li + ionic conductivity (≈1 mS cm −1 ), high shear modulus (≈55 GPa), and wide electrochemical stability window. [ 4 ] To pair the GSEs with lithium anode, quite a few approaches have been used to reduce the interfacial impedance and ensure homogeneous Li dissolution/deposition between GSEs and Li metal, including surface coating (e.g., Al 2 O 3 , [ 4,13 ] Mg, [ 14 ] graphite, [ 15 ] polymers, [ 16 ] etc.)…”

Section: Figurementioning

confidence: 99%

Tuning the Anode–Electrolyte Interface Chemistry for Garnet‐Based Solid‐State Li Metal Batteries

et al. 2020

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Lithium (Li) metal is a promising candidate as the anode for high‐energy‐density solid‐state batteries. However, interface issues, including large interfacial resistance and the generation of Li dendrites, have always frustrated the attempt to commercialize solid‐state Li metal batteries (SSLBs). Here, it is reported that infusing garnet‐type solid electrolytes (GSEs) with the air‐stable electrolyte Li3PO4 (LPO) dramatically reduces the interfacial resistance to ≈1 Ω cm2 and achieves a high critical current density of 2.2 mA cm−2 under ambient conditions due to the enhanced interfacial stability to the Li metal anode. The coated and infused LPO electrolytes not only improve the mechanical strength and Li‐ion conductivity of the grain boundaries, but also form a stable Li‐ion conductive but electron‐insulating LPO‐derived solid‐electrolyte interphase between the Li metal and the GSE. Consequently, the growth of Li dendrites is eliminated and the direct reduction of the GSE by Li metal over a long cycle life is prevented. This interface engineering approach together with grain‐boundary modification on GSEs represents a promising strategy to revolutionize the anode–electrolyte interface chemistry for SSLBs and provides a new design strategy for other types of solid‐state batteries.

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Section: Figurementioning

confidence: 99%

Tuning the Anode–Electrolyte Interface Chemistry for Garnet‐Based Solid‐State Li Metal Batteries

et al. 2020

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“…An experimental progress was reported where ultrathin Al 2 O 3 was found to significantly decrease the Li/garnet interfacial impedance from 1710 to 1 Ω cm 2 , but the current density of the corresponding symmetric cells is 0.2 mA cm −2 10a. Other surface modification approaches have been proposed and different interlayer materials such as Al, Sn, C, Si, MoS 2 , have been trialed with similar purpose 6,8,10a,c,d,17,18. In spite of all these efforts, to the best of our knowledge, the highest reported CCD value of planar lithium–garnets is still less than 0.9 mA cm −2 at room temperature .…”

Section: Introductionmentioning

confidence: 97%

“…One of the major challenges facing Li/LLZO interfaces is the sluggish Li‐ion transport across the interface signified by a large interfacial resistance . This is partially related to the poor physical contact for the solid‐solid Li/LLZO interface .…”

Section: Introductionmentioning

confidence: 99%

“…Other surface modification approaches have been proposed and different interlayer materials such as Al, Sn, C, Si, MoS 2 , have been trialed with similar purpose 6,8,10a,c,d,17,18. In spite of all these efforts, to the best of our knowledge, the highest reported CCD value of planar lithium–garnets is still less than 0.9 mA cm −2 at room temperature . By contrast, the CCD of liquid electrolytes can reach 4–10 mA cm −2 at room temperature .…”

Section: Introductionmentioning

confidence: 99%

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Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Zheng

Tian

et al. 2019

Adv Funct Materials

128

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Solid-state lithium batteries are widely considered as next-generation lithiumion battery technology due to the potential advantages in safety and performance. Among the various solid electrolyte materials, Li-garnet electrolytes are promising due to their high ionic conductivity and good chemical and electrochemical stabilities. However, the high electrode/electrolyte interfacial impedance is one of the major challenges. Moreover, short circuiting caused by lithium dendrite formation is reported when using Li-garnet electrolytes. Here, it is demonstrated that Li-garnet electrolytes wet well with lithium metal by removing the intrinsic impurity layer on the surface of the lithium metal. The Li/garnet interfacial impedance is determined to be 6.95 Ω cm 2 at room temperature. Lithium symmetric cells based on the Li-garnet electrolytes are cycled at room temperature for 950 h and current density as high as 13.3 mA cm −2 without showing signs of short circuiting. Experimental and computational results reveal that it is the surface oxide layer on the lithium metal together with the garnet surface that majorly determines the Li/garnet interfacial property. These findings suggest that removing the superficial impurity layer on the lithium metal can enhance the wettability, which may impact the manufacturing process of future high energy density garnet-based solid-state lithium batteries. are gratefully acknowledged for assisting with relevant experimental analysis. Center for High Performance Computing of SJTU is gratefully acknowledged for providing computational facilities for all the simulations. Conflict of InterestThe authors declare no conflict of interest.

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“…Due to their potential to enable Li metal anodes, significant effort has been made to study and stabilize the Li metal–solid electrolyte interface . With recent progress in this area, studies have demonstrated stable cycling of Li in a variety of solid electrolytes, ranging from oxides, to sulfides, to polymers, at current densities nearing the targets for electric vehicles (>1 mA cm −2 ). However, despite the significant progress in integrating Li metal with solid electrolytes, there has been a lack of emphasis on cathode integration.…”

Section: Introductionmentioning

confidence: 99%

Mixed Electronic and Ionic Conduction Properties of Lithium Lanthanum Titanate

Wang

Wolfenstine

Sakamoto

2020

Adv Funct Materials

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With the continued increase in Li‐metal anode rate capability, there is an equally important need to develop high‐rate cathode architectures for solid‐state batteries. A proposed method of improving charge transport in the cathode is introducing a mixed electronic and ionic conductor (MEIC) which can eliminate the need for conductive additives that occlude electrolyte–electrode interfaces and lower the net additive required in the cathode. This study takes advantage of a reduced perovskite electrolyte, Li0.33La0.57TiO3 (LLTO), to act as a model MEIC. It is found that the ionic conductivity of reduced LLTO is comparable to oxidized LLTO (σbulk = 10−3–10−4 S cm−1, σGB = 10−5–10−6 S cm−1) and the electronic conductivity is 1 mS cm−1. The ionic transference numbers are 0.9995 and 0.0095 in the oxidized and reduced state, respectively. Furthermore, two methods for controlling the transference numbers are evaluated. It is found that the electronic conductivity cannot easily be controlled by changing O2 overpressures, but increasing the ionic conductivity can be achieved by increasing grain size. This work identifies a possible class of MEIC materials that may improve rate capabilities of cathodes in solid‐state architectures and motivate a deeper understanding of MEICs in the context of solid‐state batteries.

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Demonstration of high current densities and extended cycling in the garnet Li7La3Zr2O12 solid electrolyte

Cited by 147 publications

References 23 publications

Tuning the Anode–Electrolyte Interface Chemistry for Garnet‐Based Solid‐State Li Metal Batteries

Tuning the Anode–Electrolyte Interface Chemistry for Garnet‐Based Solid‐State Li Metal Batteries

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Mixed Electronic and Ionic Conduction Properties of Lithium Lanthanum Titanate

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