Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements

AbstractA key challenge for solid-state-batteries development is to design electrode-electrolyte interfaces that combine (electro)chemical and mechanical stability with facile Li-ion transport. However, while the solid-electrolyte/electrode interfacial area should be maximized to facilitate the transport of high electrical currents on the one hand, on the other hand, this area should be minimized to reduce the parasitic interfacial reactions and promote the overall cell stability. To improve these aspects simultaneously, we report the use of an interfacial inorganic coating and the study of its impact on the local Li-ion transport over the grain boundaries. Via exchange-NMR measurements, we quantify the equilibrium between the various phases present at the interface between an S-based positive electrode and an inorganic solid-electrolyte. We also demonstrate the beneficial effect of the LiI coating on the all-solid-state cell performances, which leads to efficient sulfur activation and prevention of solid-electrolyte decomposition. Finally, we report 200 cycles with a stable capacity of around 600 mAh g−1 at 0.264 mA cm−2 for a full lab-scale cell comprising of LiI-coated Li2S-based cathode, Li-In alloy anode and Li6PS5Cl solid electrolyte.

Download Full-text

Quantifying the local Li-ion diffusion over the grain boundaries of a protective coating, revealing the impact on the macroscopic Li-ion transport in an all-solid-state battery

10.21203/rs.3.rs-309949/v1 ◽

2021 ◽

Author(s):

Ming Liu ◽

Chao Wang ◽

Chenglong Zhao ◽

Eveline van der Maas ◽

Kui Lin ◽

...

Keyword(s):

Solid State ◽

Ion Transport ◽

Solid Electrolyte ◽

Grain Boundaries ◽

Mechanical Stability ◽

Interface Reactions ◽

Conflicting Demands ◽

Solid State Batteries ◽

Li Ion ◽

The Impact

Abstract The key challenge for solid-state-batteries is to design electrode-electrolyte interfaces that combine (electro)chemical and mechanical stability with facile Li-ion transport. Typically, this presents conflicting demands, the solid electrolyte-electrode interface-area should be maximized to facilitate high currents, while it should be minimized to reduce the parasitic interface reactions and enhance stability. Addressing these issues would greatly benefit from establishing the impact of interface coatings on local Li-ion transport over the grain boundaries. Here, the three-phase Li-ion transport, between solid electrolyte, coating and electrode is revealed using exchange-NMR, disentangling the detailed quantitative impact of the coating on the Li-ion transport in solid state batteries. A Li2S cathode is coated by LiI, providing a ductile and conductive interface with the argyrodite-sulfur electrolyte, where the exchange-NMR demonstrates that this enhances the interface transport to such an extent that the commonly applied nanosizing of the cathodic mixture can be abandoned. This leads to facile sulfur activation, preventing solid-electrolyte decomposition, in micron-sized cathodic mixtures, that can be related to the role of coatings on the Li-ion transport, providing perspectives for sulfur based solid-state-batteries.

Download Full-text

Quantifying the impact of disorder on Li-ion and Na-ion transport in perovskite titanate solid electrolytes for solid-state batteries

Journal of Materials Chemistry A ◽

10.1039/d0ta05343k ◽

2020 ◽

Vol 8 (37) ◽

pp. 19603-19611

Author(s):

Adam R. Symington ◽

John Purton ◽

Joel Statham ◽

Marco Molinari ◽

M. Saiful Islam ◽

...

Keyword(s):

Solid State ◽

Ion Transport ◽

Solid Electrolytes ◽

Research Interest ◽

Considerable Research ◽

Solid State Batteries ◽

Li Ion ◽

All Solid State Batteries ◽

And Performance ◽

The Impact

Solid electrolytes for all-solid-state batteries are generating considerable research interest as a means to improving their safety, stability and performance.

Download Full-text

Reduced Sintering Temperatures of Li+ Conductive Li1.3Al0.3Ti1.7(PO4)3 Ceramics

Crystals ◽

10.3390/cryst10050408 ◽

2020 ◽

Vol 10 (5) ◽

pp. 408

Author(s):

Katja Waetzig ◽

Christian Heubner ◽

Mihails Kusnezoff

Keyword(s):

Solid State ◽

Ionic Conductivity ◽

Cathode Material ◽

Solid Electrolyte ◽

Composite Cathode ◽

Li Ion Batteries ◽

Promising Candidate ◽

Composite Cathodes ◽

Solid State Batteries ◽

Li Ion

All-solid-state batteries (ASSB) are considered promising candidates for future energy storage and advanced electric mobility. When compared to conventional Li-ion batteries, the substitution of Li-ion conductive, flammable liquids by a solid electrolyte and the application of Li-metal anodes substantially increase safety and energy density. The solid electrolyte Li1.3Al0.3Ti1.7(PO4)3 (LATP) provides high Li-ion conductivity of about 10−3 S/cm and is considered a highly promising candidate for both the solid electrolyte-separator and the ionically conductive part of the all-solid state composite cathode, consisting of the cathode material, the solid electrolyte, and an electron conductor. Co-sintering of the composite cathode is a sophisticated challenge, because temperatures above 1000 °C are typically required to achieve the maximum ionic conductivity of LATP but provoke reactions with the cathode material, inhibiting proper electrochemical functioning in the ASSB. In the present study, the application of sintering aids with different melting points and their impact on the sinterability and the conductivity of LATP were investigated by means of optical dilatometry and impedance spectroscopy. The microstructure of the samples was analyzed by SEM. The results indicate that the sintering temperature can be reduced below 800 °C while maintaining high ionic conductivity of up to 3.6 × 10−4 S/cm. These insights can be considered a crucial step forward towards enable LATP-based composite cathodes for future ASSB.

Download Full-text

Operando Neutron Imaging for Next-Generation Solid State Batteries: A Direct Visualization of Li-Ion Transport in Sulfide Materials

ECS Meeting Abstracts ◽

10.1149/ma2019-03/2/226 ◽

2019 ◽

Keyword(s):

Solid State ◽

Ion Transport ◽

Neutron Imaging ◽

Direct Visualization ◽

Next Generation ◽

Solid State Batteries ◽

Li Ion

Download Full-text

Revealing the Impact of Space-Charge Layers on the Li-Ion Transport in All-Solid-State Batteries

Joule ◽

10.1016/j.joule.2020.04.002 ◽

2020 ◽

Vol 4 (6) ◽

pp. 1311-1323 ◽

Cited By ~ 3

Author(s):

Zhu Cheng ◽

Ming Liu ◽

Swapna Ganapathy ◽

Chao Li ◽

Zhaolong Li ◽

...

Keyword(s):

Solid State ◽

Ion Transport ◽

Space Charge ◽

Solid State Batteries ◽

Li Ion ◽

All Solid State Batteries ◽

The Impact

Download Full-text

In-situ electron holography charactering Li ions accumulation in the interface between electrode and solid-state-electrolyte

Journal of Materials Chemistry A ◽

10.1039/d1ta03517g ◽

2021 ◽

Author(s):

Yang Yang ◽

Jie Cui ◽

Hui-Juan Guo ◽

Xi Shen ◽

Yuan Yao ◽

...

Keyword(s):

Solid State ◽

Ion Transport ◽

Charge Distribution ◽

Transport Mechanism ◽

Electron Holography ◽

Solid State Electrolyte ◽

Solid State Batteries ◽

Li Ion ◽

Solid State Electrolytes

Intensive understanding of the Li-ion transport mechanism in solid-state-electrolytes (SSEs) is crucial for the buildup of industrially scalable solid-state batteries. Here, we report the charge distribution near the electrode/SSEs interface...

Download Full-text