Review on the lithium transport mechanism in solid‐state battery materials

Abstract

The growing demands to mitigate climate change and environmental degradation stimulate the rapid developments of rechargeable lithium (Li) battery technologies. Fast Li transports in battery materials are of essential significance to ensure superior Li dynamical stability and rate performance of batteries. Herein, the Li transport mechanisms in solid‐state battery materials (SSBMs) are comprehensively summarized. The collective diffusion mechanisms in solid electrolytes are elaborated, which are further understood from multiple perspectives including lattice dynamics, crystalline structure, and electronic structure. With the exponentially improving performance of computers, atomistic simulations have been playing an increasingly important role in revealing and understanding the Li transport in SSBMs, bridging the gap between experimental phenomena and theoretical models. Theoretical and experimental characterization methods for Li transports are discussed. The design strategies toward fast Li transports are classified. Finally, a perspective on the achievements and challenges of probing Li transports is provided. This article is categorized under: Structure and Mechanism > Computational Materials Science

Unravelling the alkali transport properties in nanocrystalline A3OX (A = Li, Na, X = Cl, Br) solid state electrolytes. A theoretical prediction

“…The search for affordable inorganic electrolytes for future all solid state alkali-ion batteries is one of the current hot topics due to the urgent need for high energy density materials and relevant safety issues. [1][2][3][4][5] Exploration and prediction of the properties of electrolytes are crucial for the improvement of performance and durability of the battery. [1][2][3][4][5][6][7] Of particular interest, the development of inorganic solid electrolyte faces critical issues, such as the lower electrical conductivity as compared to conventional liquid electrolytes, interfacial resistance with the electrodes, narrow electrochemical window that constrain its practical applications.…”

“…[1][2][3][4][5] Exploration and prediction of the properties of electrolytes are crucial for the improvement of performance and durability of the battery. [1][2][3][4][5][6][7] Of particular interest, the development of inorganic solid electrolyte faces critical issues, such as the lower electrical conductivity as compared to conventional liquid electrolytes, interfacial resistance with the electrodes, narrow electrochemical window that constrain its practical applications. [4][5][6][7] Of the compounds with special interest for inorganic solid electrolyte, the Li-rich anti-perovskite Li 3 OX (X ¼ Cl À , Br À ) has attracted large scientic interest due to the high Li ionic conductivity (z1 mS cm À1 ) and stability with the electrode, and low Li activation energy (z0.2 eV).…”

“…[1][2][3][4][5][6][7] Of particular interest, the development of inorganic solid electrolyte faces critical issues, such as the lower electrical conductivity as compared to conventional liquid electrolytes, interfacial resistance with the electrodes, narrow electrochemical window that constrain its practical applications. [4][5][6][7] Of the compounds with special interest for inorganic solid electrolyte, the Li-rich anti-perovskite Li 3 OX (X ¼ Cl À , Br À ) has attracted large scientic interest due to the high Li ionic conductivity (z1 mS cm À1 ) and stability with the electrode, and low Li activation energy (z0.2 eV). [8][9][10][11][12] Nevertheless, a higher activation energy (z0.6 eV) and a lower ionic conductivity for Li 3 OX have recently been reported experimentally.…”

“…1–5 Exploration and prediction of the properties of electrolytes are crucial for the improvement of performance and durability of the battery. 1–7 Of particular interest, the development of inorganic solid electrolyte faces critical issues, such as the lower electrical conductivity as compared to conventional liquid electrolytes, interfacial resistance with the electrodes, narrow electrochemical window that constrain its practical applications. 4–7…”

Synergy of non-lithium cation doping and the lithium concentration affecting lithium ion transport in solid electrolytes

“…Many factors have impacts on lithium-ion migration. 7,8 In addition to the arrangement of anions (body-centered cubic, face-centered cubic and hexagonal close-packed), 9,10 the unit volume of a single anion and the charge it carries, [11][12][13] and cations also possess very complex effects on lithium-ion migration. 14,15 On one hand, some literature studies report that the concentration of lithium ions itself has effects of nonlinear relationships on the diffusion of lithium ions, and there is generally an optimal lithium-ion concentration.…”