scholarly journals Insights into interfacial effect and local lithium-ion transport in polycrystalline cathodes of solid-state batteries

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Shuaifeng Lou ◽  
Qianwen Liu ◽  
Fang Zhang ◽  
Qingsong Liu ◽  
Zhenjiang Yu ◽  
...  
Keyword(s):  
Solid State ◽  
Ion Transport ◽  
Chemical Potential ◽  
Lithium Ion ◽  
Local Environment ◽  
Underlying Mechanism ◽  
Transport Kinetics ◽  
Potential Force ◽  
Interfacial Contact ◽  
Solid State Batteries

Abstract Interfacial issues commonly exist in solid-state batteries, and the microstructural complexity combines with the chemical heterogeneity to govern the local interfacial chemistry. The conventional wisdom suggests that “point-to-point” ion diffusion at the interface determines the ion transport kinetics. Here, we show that solid-solid ion transport kinetics are not only impacted by the physical interfacial contact but are also closely associated with the interior local environments within polycrystalline particles. In spite of the initial discrete interfacial contact, solid-state batteries may still display homogeneous lithium-ion transportation owing to the chemical potential force to achieve an ionic-electronic equilibrium. Nevertheless, once the interior local environment within secondary particle is disrupted upon cycling, it triggers charge distribution from homogeneity to heterogeneity and leads to fast capacity fading. Our work highlights the importance of interior local environment within polycrystalline particles for electrochemical reactions in solid-state batteries and provides crucial insights into underlying mechanism in interfacial transport.

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>

Dendrites in Solid‐State Batteries: Ion Transport Behavior, Advanced Characterization, and Interface Regulation

2021 ◽  
pp. 2003250
Author(s):  
Zhenjiang Yu ◽  
Xueyan Zhang ◽  
Chuankai Fu ◽  
Han Wang ◽  
Ming Chen ◽  
...  
Keyword(s):  
Solid State ◽  
Ion Transport ◽  
Advanced Characterization ◽  
Transport Behavior ◽  
Solid State Batteries

Enhancing interfacial contact in all solid state batteries with a cathode-supported solid electrolyte membrane framework

2019 ◽  
Vol 12 (3) ◽  
pp. 938-944 ◽  
Author(s):  
Xinzhi Chen ◽  
Wenjun He ◽  
Liang-Xin Ding ◽  
Suqing Wang ◽  
Haihui Wang
Keyword(s):  
Solid State ◽  
Electrochemical Performance ◽  
Solid Electrolyte ◽  
Electrolyte Membrane ◽  
Interfacial Contact ◽  
Solid State Batteries ◽  
All Solid State Batteries

A cathode-supported solid electrolyte membrane framework with enhanced interfacial contact can significantly improve the electrochemical performance of all solid state batteries.

scholarly journals All-Solid-State Lithium Ion Batteries Using Self-Organized TiO2 Nanotubes Grown from Ti-6Al-4V Alloy

Molecules ◽  
2020 ◽  
Vol 25 (9) ◽  
pp. 2121
Author(s):  
Vinsensia Ade Sugiawati ◽  
Florence Vacandio ◽  
Thierry Djenizian
Keyword(s):  
Cyclic Voltammetry ◽  
Solid State ◽  
Tio2 Nanotubes ◽  
Coulombic Efficiency ◽  
Lithium Ion ◽  
Electrochemical Anodization ◽  
Self Organized ◽  
Solid State Batteries ◽  
One Step ◽  
Tio2 Nts

All-solid-state batteries were fabricated by assembling a layer of self-organized TiO2 nanotubes grown on as anode, a thin-film of polymer as an electrolyte and separator, and a layer of composite LiFePO4 as a cathode. The synthesis of self-organized TiO2 NTs from Ti-6Al-4V alloy was carried out via one-step electrochemical anodization in a fluoride ethylene glycol containing electrolytes. The electrodeposition of the polymer electrolyte onto anatase TiO2 NTs was performed by cyclic voltammetry. The anodized Ti-6Al-4V alloys were characterized by scanning electron microscopy and X-ray diffraction. The electrochemical properties of the anodized Ti-6Al-4V alloys were investigated by cyclic voltammetry and chronopotentiometry techniques. The full-cell shows a high first-cycle Coulombic efficiency of 96.8% with a capacity retention of 97.4% after 50 cycles and delivers a stable discharge capacity of 63 μAh cm−2 μm−1 (119 mAh g−1) at a kinetic rate of C/10.

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