Dataset Information

A Two-Parameter Space to Tune Solid Electrolytes for Lithium Dendrite Constriction.

ABSTRACT: Li dendrite penetration, and associated microcrack propagation, at high current densities is one main challenge to the stable cycling of solid-state batteries. The interfacial decomposition reaction between Li dendrite and a solid electrolyte was recently used to suppress Li dendrite penetration through a novel effect of "dynamic stability". Here we use a two-parameter space to classify electrolytes and propose that the effect may require the electrolyte to occupy a certain region in the space, with the principle of delicately balancing the two property metrics of a sufficient decomposition energy with the Li metal and a low critical mechanical modulus. Furthermore, in our computational prediction prepared using a combination of high-throughput computation and machine learning, we show that the positions of electrolytes in such a space can be controlled by the chemical composition of the electrolyte; the compositions can also be attained by experimental synthesis using core-shell microstructures. The designed electrolytes following this principle further demonstrate stable long cycling from 10 000 to 20 000 cycles at high current densities of 8.6-30 mA/cm² in solid-state batteries, while in contrast the control electrolyte with a nonideal position in the two-parameter space showed a capacity decay that was faster by at least an order of magnitude due to Li dendrite penetration.

SUBMITTER: Wang Y

PROVIDER: S-EPMC9088294 | biostudies-literature | 2022 Apr

REPOSITORIES: biostudies-literature

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A Two-Parameter Space to Tune Solid Electrolytes for Lithium Dendrite Constriction.

Wang Yichao Y Ye Luhan L Chen Xi X Li Xin X

JACS Au 20220329 4

Li dendrite penetration, and associated microcrack propagation, at high current densities is one main challenge to the stable cycling of solid-state batteries. The interfacial decomposition reaction between Li dendrite and a solid electrolyte was recently used to suppress Li dendrite penetration through a novel effect of "dynamic stability". Here we use a two-parameter space to classify electrolytes and propose that the effect may require the electrolyte to occupy a certain region in the space, ...[more]

PMID: 35557758

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Project description:Next generation batteries based on lithium (Li) metal anodes have been plagued by the dendritic electrodeposition of Li metal on the anode during cycling, resulting in short circuit and capacity loss. Suppression of dendritic growth through the use of solid electrolytes has emerged as one of the most promising strategies for enabling the use of Li metal anodes. We perform a computational screening of over 12 000 inorganic solids based on their ability to suppress dendrite initiation in contact with Li metal anode. Properties for mechanically isotropic and anisotropic interfaces that can be used in stability criteria for determining the propensity of dendrite initiation are usually obtained from computationally expensive first-principles methods. In order to obtain a large data set for screening, we use machine-learning models to predict the mechanical properties of several new solid electrolytes. The machine-learning models are trained on purely structural features of the material, which do not require any first-principles calculations. We train a graph convolutional neural network on the shear and bulk moduli because of the availability of a large training data set with low noise due to low uncertainty in their first-principles-calculated values. We use gradient boosting regressor and kernel ridge regression to train the elastic constants, where the choice of the model depends on the size of the training data and the noise that it can handle. The material stiffness is found to increase with an increase in mass density and ratio of Li and sublattice bond ionicity, and decrease with increase in volume per atom and sublattice electronegativity. Cross-validation/test performance suggests our models generalize well. We predict over 20 mechanically anisotropic interfaces between Li metal and four solid electrolytes which can be used to suppress dendrite growth. Our screened candidates are generally soft and highly anisotropic, and present opportunities for simultaneously obtaining dendrite suppression and high ionic conductivity in solid electrolytes.

Dataset Information

A Two-Parameter Space to Tune Solid Electrolytes for Lithium Dendrite Constriction.

Publications

A Two-Parameter Space to Tune Solid Electrolytes for Lithium Dendrite Constriction.

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