scholarly journals Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li7La3Zr2O12 Solid Electrolytes

Materials ◽  
2021 ◽  
Vol 14 (22) ◽  
pp. 6809
Author(s):  
Markus Mann ◽  
Michael Küpers ◽  
Grit Häuschen ◽  
Martin Finsterbusch ◽  
Dina Fattakhova-Rohlfing ◽  
...  
Keyword(s):  
Solid State ◽  
Solid Electrolyte ◽  
Spray Drying ◽  
Solid State Reaction ◽  
High Energy ◽  
Cubic Phase ◽  
Synthesis Methods ◽  
Wet Chemical Synthesis ◽  
Solid State Batteries ◽  
Co Precipitation

Solid electrolyte is the key component in all-solid-state batteries (ASBs). It is required in electrodes to enhance Li-conductivity and can be directly used as a separator. With its high Li-conductivity and chemical stability towards metallic lithium, lithium-stuffed garnet material Li7La3Zr2O12 (LLZO) is considered one of the most promising solid electrolyte materials for high-energy ceramic ASBs. However, in order to obtain high conductivities, rare-earth elements such as tantalum or niobium are used to stabilize the highly conductive cubic phase. This stabilization can also be obtained via high levels of aluminum, reducing the cost of LLZO but also reducing processability and the Li-conductivity. To find the sweet spot for a potential market introduction of garnet-based solid-state batteries, scalable and industrially usable syntheses of LLZO with high processability and good conductivity are indispensable. In this study, four different synthesis methods (solid-state reaction (SSR), solution-assisted solid-state reaction (SASSR), co-precipitation (CP), and spray-drying (SD)) were used and compared for the synthesis of aluminum-substituted LLZO (Al:LLZO, Li6.4Al0.2La3Zr2O12), focusing on electrochemical performance on the one hand and scalability and environmental footprint on the other hand. The synthesis was successful via all four methods, resulting in a Li-ion conductivity of 2.0–3.3 × 10−4 S/cm. By using wet-chemical synthesis methods, the calcination time could be reduced from two calcination steps for 20 h at 850 °C and 1000 °C to only 1 h at 1000 °C for the spray-drying method. We were able to scale the synthesis up to a kg-scale and show the potential of the different synthesis methods for mass production.

Enhancing the polymer electrolyte – Li metal interface on high-voltage solid-state batteries with Li-based additives inspired by the surface chemistry of Li7La3Zr2012

2022 ◽  
Author(s):  
Ander Orue ◽  
Mikel Arrese-Igor ◽  
Rosalía Cid ◽  
Xabier Judez ◽  
Nuria Gómez ◽  
...  
Keyword(s):  
Solid State ◽  
Surface Chemistry ◽  
Solid Electrolyte ◽  
Polymer Electrolyte ◽  
Power Density ◽  
High Voltage ◽  
High Energy ◽  
Metal Interface ◽  
Solid State Batteries ◽  
Energy And Power Density

High-voltage Li metal solid-state batteries are in the spotlight of high energy and power density devices for the next generation of batteries. However, the lack of robust solid-electrolyte interfaces (SEI)...

Integrated cathode and solid electrolyte via in situ polymerization with significantly reduced interface resistance

2021 ◽  
Author(s):  
Jialiang Yuan ◽  
Ran Dong ◽  
Yuan Li ◽  
Yang Liu ◽  
Zhuo Zheng ◽  
...  
Keyword(s):  
Solid State ◽  
Energy Density ◽  
Solid Electrolyte ◽  
In Situ Polymerization ◽  
High Energy ◽  
High Energy Density ◽  
Interface Resistance ◽  
Simple Strategy ◽  
Solid State Batteries

Reducing the interface resistance of solid electrolyte and electrode is critical for developing high-energy density solid-state batteries. In the present study, a simple strategy that designing integrated cathode and solide...

Electrochemical properties of all-solid-state lithium secondary batteries using Li-argyrodite Li6PS5Cl as solid electrolyte

2013 ◽  
Vol 1496 ◽  
Author(s):  
Sylvain Boulineau ◽  
Jean-Marie Tarascon ◽  
Vincent Seznec ◽  
Virginie Viallet
Keyword(s):  
Solid State ◽  
Electrochemical Properties ◽  
Solid Electrolyte ◽  
Active Material ◽  
Reversible Capacity ◽  
High Energy ◽  
Electrochemical Stability ◽  
Lithium Secondary Batteries ◽  
Solid State Batteries ◽  
Energy Ball

ABSTRACTHighly ion-conductive Li6PS5Cl Li-argyrodites were prepared through a high energy ball milling. Electrical and electrochemical properties were investigated. Ball-milled compounds exhibit a high conductivity of 1.33×10−4 S/cm with an activation energy of 0.3-0.4 eV and an electrochemical stability up to 7V vs. lithium. These results are obtained after only 10 hours of milling and with no additional heat treatment.To validate the use of the Li6PS5Cl-based solid electrolyte, all-solid-state batteries using LiCoO2 and Li4Ti5O12 as active material have been realized. The optimization of the electrode composition led to a maximum of 46 and 27 mAh per gram of composite for LiCoO2 and Li4Ti5O12-based half-cells respectively. The assembled all-solid-state LiCoO2 / Li6PS5Cl / Li4Ti5O12 battery presents a sustainable reversible capacity of 27 mAh per gram of active material and a coulomb efficiency close to 99%.

scholarly journals Preparation and Application of Garnet Electrolyte Thin Films: Promise and Challenges

2020 ◽  
pp. 6-22 ◽  
Author(s):  
Xufeng Yan ◽  
Weiqiang Han
Keyword(s):  
Thin Film ◽  
Solid State ◽  
Energy Density ◽  
Solid Electrolyte ◽  
High Energy ◽  
High Energy Density ◽  
Electrochemical Performances ◽  
Safety Property ◽  
Solid State Batteries ◽  
All Solid State Batteries

All-solid-state batteries (ASSBs) have attracted much attention in recent years, due to their high energy density, excellent cycling performance, and superior safety property. As the key factor of all-solid-state batteries, solid electrolyte determines the performance of the batteries. Garnet-typed cubic Li7La3Zr2O12(LLZO) has been reported as the most promising solid electrolyte on the way to ASSBs. Thin film electrolyte could contribute to a higher energy density and a lower resistance in a battery. This short review exhibits the latest efforts on LLZO thin film and discusses the different preparation methods, together with their effects on characteristics and electrochemical performances of the solid electrolyte film.

scholarly journals Current Status and Prospects of Solid-State Batteries as the Future of Energy Storage

2021 ◽  
Author(s):  
Marm Dixit ◽  
Nitin Muralidharan ◽  
Anand Parejiya ◽  
Ruhul Amin ◽  
Rachid Essehli ◽  
...  
Keyword(s):  
Energy Storage ◽  
Solid State ◽  
Solid Electrolyte ◽  
High Capacity ◽  
Lithium Ion ◽  
High Energy ◽  
Current Status ◽  
Solid State Battery ◽  
Solid State Batteries ◽  
And Performance

Solid-state battery (SSB) is the new avenue for achieving safe and high energy density energy storage in both conventional but also niche applications. Such batteries employ a solid electrolyte unlike the modern-day liquid electrolyte-based lithium-ion batteries and thus facilitate the use of high-capacity lithium metal anodes thereby achieving high energy densities. Despite this promise, practical realization and commercial adoption of solid-state batteries remain a challenge due to the underlying material and cell level issues that needs to be overcome. This chapter thus covers the specific challenges, design principles and performance improvement strategies pertaining to the cathode, solid electrolyte and anode used in solid state batteries. Perspectives and outlook on specific applications that can benefit from the successful implementation of solid-state battery systems are also discussed. Overall, this chapter highlights the potential of solid-state batteries for successful commercial deployment in next generation energy storage systems.

scholarly journals Li1.5La1.5MO6 (M = W6+, Te6+) as a new series of lithium-rich double perovskites for all-solid-state lithium-ion batteries

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Marco Amores ◽  
Hany El-Shinawi ◽  
Innes McClelland ◽  
Stephen R. Yeandel ◽  
Peter J. Baker ◽  
...  
Keyword(s):  
Solid State ◽  
Solid Electrolyte ◽  
Specific Capacity ◽  
Lithium Ion ◽  
High Energy ◽  
Double Perovskites ◽  
Structure Property ◽  
Ion Diffusion ◽  
Ion Distribution ◽  
Solid State Batteries

AbstractSolid-state batteries are a proposed route to safely achieving high energy densities, yet this architecture faces challenges arising from interfacial issues between the electrode and solid electrolyte. Here we develop a novel family of double perovskites, Li1.5La1.5MO6 (M = W6+, Te6+), where an uncommon lithium-ion distribution enables macroscopic ion diffusion and tailored design of the composition allows us to switch functionality to either a negative electrode or a solid electrolyte. Introduction of tungsten allows reversible lithium-ion intercalation below 1 V, enabling application as an anode (initial specific capacity >200 mAh g-1 with remarkably low volume change of ∼0.2%). By contrast, substitution of tungsten with tellurium induces redox stability, directing the functionality of the perovskite towards a solid-state electrolyte with electrochemical stability up to 5 V and a low activation energy barrier (<0.2 eV) for microscopic lithium-ion diffusion. Characterisation across multiple length- and time-scales allows interrogation of the structure-property relationships in these materials and preliminary examination of a solid-state cell employing both compositions suggests lattice-matching avenues show promise for all-solid-state batteries.

Rational Design of Quasi Zero-Strain NCM Cathode Materials for Minimizing Volume Change Effects in All-Solid-State Batteries

2019 ◽  
Author(s):  
Florian Strauss ◽  
Lea de Biasi ◽  
A-Young Kim ◽  
Jonas Hertle ◽  
Simon Schweidler ◽  
...  
Keyword(s):  
Solid State ◽  
Solid Electrolyte ◽  
Cathode Materials ◽  
Rational Design ◽  
Electrode Materials ◽  
Cycling Performance ◽  
Mechanical Degradation ◽  
Volume Changes ◽  
Solid State Batteries ◽  
All Solid State Batteries

Measures to improve the cycling performance and stability of bulk-type all-solid-state batteries (SSBs) are currently being developed with the goal of substituting conventional Li-ion battery (LIB) technology. As known from liquid electrolyte based LIBs, layered oxide cathode materials undergo volume changes upon (de)lithiation, causing mechanical degradation due to particle fracture, among others. Unlike solid electrolytes, liquid electrolytes are somewhat capable of accommodating morphological changes. In SSBs, the rigidity of the materials used typically leads to adverse contact loss at the interfaces of cathode material and solid electrolyte during cycling. Hence, designing zero- or low-strain electrode materials for application in next-generation SSBs is desirable. In the present work, we report on novel Co-rich NCMs, NCM361 (60% Co) and NCM271 (70% Co), showing minor volume changes up to 4.5 V vs Li<sup>+</sup>/Li, as determined by <i>operando</i> X-ray diffraction and pressure measurements of LIB pouch and pelletized SSB cells, respectively. Both cathode materials exhibit good cycling performance when incorporated into SSB cells using argyrodite Li<sub>6</sub>PS<sub>5</sub>Cl solid electrolyte, albeit their morphology and secondary particle size have not yet been optimized.

Rational Design of Quasi Zero-Strain NCM Cathode Materials for Minimizing Volume Change Effects in All-Solid-State Batteries

2019 ◽  
Author(s):  
Florian Strauss ◽  
Lea de Biasi ◽  
A-Young Kim ◽  
Jonas Hertle ◽  
Simon Schweidler ◽  
...  
Keyword(s):  
Solid State ◽  
Solid Electrolyte ◽  
Cathode Materials ◽  
Rational Design ◽  
Electrode Materials ◽  
Cycling Performance ◽  
Mechanical Degradation ◽  
Volume Changes ◽  
Solid State Batteries ◽  
All Solid State Batteries

Measures to improve the cycling performance and stability of bulk-type all-solid-state batteries (SSBs) are currently being developed with the goal of substituting conventional Li-ion battery (LIB) technology. As known from liquid electrolyte based LIBs, layered oxide cathode materials undergo volume changes upon (de)lithiation, causing mechanical degradation due to particle fracture, among others. Unlike solid electrolytes, liquid electrolytes are somewhat capable of accommodating morphological changes. In SSBs, the rigidity of the materials used typically leads to adverse contact loss at the interfaces of cathode material and solid electrolyte during cycling. Hence, designing zero- or low-strain electrode materials for application in next-generation SSBs is desirable. In the present work, we report on novel Co-rich NCMs, NCM361 (60% Co) and NCM271 (70% Co), showing minor volume changes up to 4.5 V vs Li<sup>+</sup>/Li, as determined by <i>operando</i> X-ray diffraction and pressure measurements of LIB pouch and pelletized SSB cells, respectively. Both cathode materials exhibit good cycling performance when incorporated into SSB cells using argyrodite Li<sub>6</sub>PS<sub>5</sub>Cl solid electrolyte, albeit their morphology and secondary particle size have not yet been optimized.

Experimental Assessment of the Practical Oxidative Stability of Lithium Thiophosphate Solid Electrolytes

2019 ◽  
Author(s):  
Georg Dewald ◽  
Saneyuki Ohno ◽  
Marvin Kraft ◽  
Raimund Koerver ◽  
Paul Till ◽  
...  
Keyword(s):  
Cyclic Voltammetry ◽  
Solid State ◽  
Oxidative Stability ◽  
Photoelectron Spectroscopy ◽  
Solid Electrolytes ◽  
Stability Limit ◽  
Lithium Ion ◽  
High Energy ◽  
Redox Activity ◽  
Solid State Batteries

<p>All-solid-state batteries are often expected to replace conventional lithium-ion batteries in the future. However, the practical electrochemical and cycling stability of the best-conducting solid electrolytes, i.e. lithium thiophosphates, are still critical issues that prevent long-term stable high-energy cells. In this study, we use <i>stepwise</i><i>cyclic voltammetry </i>to obtain information on the practical oxidative stability limit of Li<sub>10</sub>GeP<sub>2</sub>S<sub>12</sub>, a Li<sub>2</sub>S‑P<sub>2</sub>S<sub>5</sub>glass, as well as the argyrodite Li<sub>6</sub>PS<sub>5</sub>Cl solid electrolytes. We employ indium metal and carbon black as the counter and working electrode, respectively, the latter to increase the interfacial contact area to the electrolyte as compared to the commonly used planar steel electrodes. Using a stepwise increase in the reversal potentials, the onset potential at 25 °C of oxidative decomposition at the electrode-electrolyte interface is identified. X‑ray photoelectron spectroscopy is used to investigate the oxidation of sulfur(-II) in the thiophosphate polyanions to sulfur(0) as the dominant redox process in all electrolytes tested. Our results suggest that after the formation of these decomposition products, significant redox behavior is observed. This explains previously reported redox activity of thiophosphate solid electrolytes, which contributes to the overall cell performance in solid-state batteries. The <i>stepwise cyclic voltammetry</i>approach presented here shows that the practical oxidative stability at 25 °C of thiophosphate solid electrolytes against carbon is kinetically higher than predicted by thermodynamic calculations. The method serves as an efficient guideline for the determination of practical, kinetic stability limits of solid electrolytes. </p>

Experimental Assessment of the Practical Oxidative Stability of Lithium Thiophosphate Solid Electrolytes

2019 ◽  
Author(s):  
Georg Dewald ◽  
Saneyuki Ohno ◽  
Marvin Kraft ◽  
Raimund Koerver ◽  
Paul Till ◽  
...  
Keyword(s):  
Cyclic Voltammetry ◽  
Solid State ◽  
Oxidative Stability ◽  
Photoelectron Spectroscopy ◽  
Solid Electrolytes ◽  
Stability Limit ◽  
Lithium Ion ◽  
High Energy ◽  
Redox Activity ◽  
Solid State Batteries

<p>All-solid-state batteries are often expected to replace conventional lithium-ion batteries in the future. However, the practical electrochemical and cycling stability of the best-conducting solid electrolytes, i.e. lithium thiophosphates, are still critical issues that prevent long-term stable high-energy cells. In this study, we use <i>stepwise</i><i>cyclic voltammetry </i>to obtain information on the practical oxidative stability limit of Li<sub>10</sub>GeP<sub>2</sub>S<sub>12</sub>, a Li<sub>2</sub>S‑P<sub>2</sub>S<sub>5</sub>glass, as well as the argyrodite Li<sub>6</sub>PS<sub>5</sub>Cl solid electrolytes. We employ indium metal and carbon black as the counter and working electrode, respectively, the latter to increase the interfacial contact area to the electrolyte as compared to the commonly used planar steel electrodes. Using a stepwise increase in the reversal potentials, the onset potential at 25 °C of oxidative decomposition at the electrode-electrolyte interface is identified. X‑ray photoelectron spectroscopy is used to investigate the oxidation of sulfur(-II) in the thiophosphate polyanions to sulfur(0) as the dominant redox process in all electrolytes tested. Our results suggest that after the formation of these decomposition products, significant redox behavior is observed. This explains previously reported redox activity of thiophosphate solid electrolytes, which contributes to the overall cell performance in solid-state batteries. The <i>stepwise cyclic voltammetry</i>approach presented here shows that the practical oxidative stability at 25 °C of thiophosphate solid electrolytes against carbon is kinetically higher than predicted by thermodynamic calculations. The method serves as an efficient guideline for the determination of practical, kinetic stability limits of solid electrolytes. </p>

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