Dataset Information

Elucidating the Role of Microstructure in Thiophosphate Electrolytes - a Combined Experimental and Theoretical Study of β-Li₃ PS₄.

ABSTRACT: Solid-state batteries (SSBs) are promising candidates to significantly exceed the energy densities of today's state-of-the-art technology, lithium-ion batteries (LIBs). To enable this advancement, optimizing the solid electrolyte (SE) is the key. β-Li₃ PS₄ (β-LPS) is the most studied member of the Li₂ S-P₂ S₅ family, offering promising properties for implementation in electric vehicles. In this work, the microstructure of this SE and how it influences the electrochemical performance are systematically investigated. To figure this out, four batches of β-LPS electrolyte with different particle size, shape, and porosity are investigated in detail. It is found that differences in pellet porosities mostly originate from single-particle intrinsic features and less from interparticle voids. Surprisingly, the β-LPS electrolyte pellets with the highest porosity and larger particle size not only show the highest ionic conductivity (up to 0.049 mS cm^-1 at RT), but also the most stable cycling performance in symmetrical Li cells. This behavior is traced back to the grain boundary resistance. Larger SE particles seem to be more attractive, as their grain boundary contribution is lower than that of denser pellets prepared using smaller β-LPS particles.

SUBMITTER: Ates T

PROVIDER: S-EPMC9218768 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Publications

Elucidating the Role of Microstructure in Thiophosphate Electrolytes - a Combined Experimental and Theoretical Study of β-Li3 PS4.

Ates Tugce T Neumann Anton A Danner Timo T Latz Arnulf A Zarrabeitia Maider M Stepien Dominik D Varzi Alberto A Passerini Stefano S

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20220424 18

Solid-state batteries (SSBs) are promising candidates to significantly exceed the energy densities of today's state-of-the-art technology, lithium-ion batteries (LIBs). To enable this advancement, optimizing the solid electrolyte (SE) is the key. β-Li3 PS4 (β-LPS) is the most studied member of the Li2 S-P2 S5 family, offering promising properties for implementation in electric vehicles. In this work, the microstructure of this SE and how it ...[more]

PMID: 35466540

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Project description:Li-O2 batteries offer a high theoretical discharge capacity due to the formation of light discharged species such as Li2O2, which fill the porous positive electrode. However, in practice, it is challenging to reach the theoretical capacity and completely utilize the full electrode pore volume during discharge. With the formation of discharge products, the porous medium evolves, and the porosity and tortuosity factor of the positive electrode are altered through shrinkage and clogging of pores. A pore shrinks as solid discharge products accumulate, the pore clogging when it is filled (or when access is blocked). In this study, we investigate the structural evolution of the positive electrode through a combination of experimental and computational techniques. Pulsed field gradient nuclear magnetic resonance results show that the electrode tortuosity factor changes much faster than suggested by the Bruggeman relation (an equation that empirically links the tortuosity factor to the porosity) and that the electrolyte solvent affects the tortuosity factor evolution. The latter is ascribed to the different abilities of solvents to dissolve reaction intermediates, which leads to different discharge product particle sizes: on discharging using 0.5 M LiTFSI in dimethoxyethane, the tortuosity factor increases much faster than for discharging in 0.5 M LiTFSI in tetraglyme. The correlation between a discharge product size and tortuosity factor is studied using a pore network model, which shows that larger discharge products generate more pore clogging. The Knudsen diffusion effect, where collisions of diffusing molecules with pore walls reduce the effective diffusion coefficients, is investigated using a kinetic Monte Carlo model and is found to have an insignificant impact on the effective diffusion coefficient for molecules in pores with diameters above 5 nm, i.e., most of the pores present in the materials investigated here. As a consequence, pore clogging is thought to be the main origin of tortuosity factor evolution.

Dataset Information

Elucidating the Role of Microstructure in Thiophosphate Electrolytes - a Combined Experimental and Theoretical Study of β-Li₃ PS₄.

Publications

Elucidating the Role of Microstructure in Thiophosphate Electrolytes - a Combined Experimental and Theoretical Study of β-Li<sub>3</sub> PS<sub>4</sub>.

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