Tortuosity Effects in Garnet-Type Li7La3Zr2O12 Solid Electrolytes

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...

show abstract

Section: Lithium/garnet Interfacementioning

confidence: 99%

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

Wang

Zhu

et al. 2020

Advanced Energy Materials

View full text Add to dashboard Cite

show abstract

“…However, the presence of pores has been identified to influence transport and failure mechanisms strongly. 4,39 The sub-surface porosity maps clearly highlight the spatial microstructural variation, specifically at the interfacial regions.…”

mentioning

confidence: 99%

Synchrotron Imaging of Li Metal Anodes in Solid State Batteries Aided by Machine Learning

Dixit¹,

Verma²,

Zaman³

et al. 2020

Preprint

Self Cite

View full text Add to dashboard Cite

Reversible lithium metal anodes that can achieve high rate capabilities are necessary for next generation energy storage systems. Solid electrolyte can act as a barrier for unwanted physical and chemical decomposition that lead to unstable electrodeposition (e.g. dendrite and filament growth). The formation and growth of filaments is tied to unique chemo-mechanical properties that exists at buried solid|solid interfaces. Herein, in situ tomography of Li|LLZO|Li cells is carried out to track morphological transformations in Li metal electrodes and buried solid|solid interfaces during stripping and plating processes. Optimized experimental parameters provide high resolution, high contrast reconstructions that enable lithium metal visualization. Machine learning and image processing tools are combined to quantify changes in lithium metal during stripping and plating. The analysis enables quantifying local current densities and pore size distribution in lithium metal during cycling experiments. Hotspots in lithium metal are correlated with microstructural anisotropy in the solid electrolyte. Modeling studies show large heterogeneity in transport and mechanical properties of electrolyte at the electrode|electrolyte interfaces. Regions with lower effective properties (transport and mechanical) are nuclei for failure. Failure is attributed to microstructural heterogeneities in the solid electrolyte that lead to high local stress and flux distributions.

show abstract

“…In our all solid cell, Figure S9, Supporting Information illustrates that the extent of preferred orientation of lithium varied during cycling, which demonstrates that the local structure and the interfaces between lithium and LAGP play important role in the lithium orientation despite the exact mechanism is not clear at present. In addition the porosity of thin LAGP pellet may cause an increased tortuosity for Li + transport [ 26 ] and an uneven ionic distribution at lithium metal surface with respect to mm thick LAGP: as result the Li‐metal plating is favored along (110) direction and the global thin LAGP pellet reactivity is increased at 80 °C. Our new cell design based on a polypropylene window may help in future experiments regarding the investigation of thin lithium metal and the ceramic solid electrolyte interface.…”

Section: Resultsmentioning

confidence: 99%

Understanding the Reactivity of a Thin Li_1.5Al_0.5Ge_1.5(PO₄)₃ Solid‐State Electrolyte toward Metallic Lithium Anode

Paolella

Zhu

et al. 2020

Advanced Energy Materials

View full text Add to dashboard Cite

The thickness of solid‐state electrolytes (SSEs) significantly affects the energy density and safety performance of all‐solid‐state lithium batteries. However, a sufficient understanding of the reactivity toward lithium metal of ultrathin SSEs (<100 µm) based on NASICON remains lacking. Herein, for the first time, a self‐standing and ultrathin (70 µm) NASICON‐type Li1.5Al0.5Ge1.5(PO4)3 (LAGP) electrolyte via a scalable solution process is developed, and X‐ray photoelectron spectroscopy reveals that changes in LAGP at the metastable Li–LAGP interface during battery operation is temperature dependent. Severe germanium reduction and decrease in LAGP particle size are detected at the Li–LAGP interface at elevated temperature. Oriented plating of lithium metal on its preferred (110) face occurs during in situ X‐ray diffraction cycling.

show abstract

Tortuosity Effects in Garnet-Type Li₇La₃Zr₂O₁₂ Solid Electrolytes

Cited by 87 publications

References 64 publications

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

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

Synchrotron Imaging of Li Metal Anodes in Solid State Batteries Aided by Machine Learning

Understanding the Reactivity of a Thin Li_1.5Al_0.5Ge_1.5(PO₄)₃ Solid‐State Electrolyte toward Metallic Lithium Anode

Contact Info

Product

Resources

About

Tortuosity Effects in Garnet-Type Li7La3Zr2O12 Solid Electrolytes

Cited by 87 publications

References 64 publications

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

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

Synchrotron Imaging of Li Metal Anodes in Solid State Batteries Aided by Machine Learning

Understanding the Reactivity of a Thin Li1.5Al0.5Ge1.5(PO4)3 Solid‐State Electrolyte toward Metallic Lithium Anode

Contact Info

Product

Resources

About

Tortuosity Effects in Garnet-Type Li₇La₃Zr₂O₁₂ Solid Electrolytes

Understanding the Reactivity of a Thin Li_1.5Al_0.5Ge_1.5(PO₄)₃ Solid‐State Electrolyte toward Metallic Lithium Anode