Geometric crystal structure analysis using three-dimensional Voronoi tessellation provides intuitive insights into the ionic transport behavior of metal-ion electrode materials or solid electrolytes by mapping the void space in a framework onto a network. The existing tools typically consider only the local voids by mapping them with Voronoi polyhedra vertices and then define the mobile ions pathways using the Voronoi edges connecting these vertices. We show that in some structures mobile ions are located on Voronoi polyhedra faces and thus cannot be located by a standard approach. To address this deficiency, we extend the method to include Voronoi faces in the constructed network. This method has been implemented in the CAVD python package. Its effectiveness is demonstrated by 99% recovery rate for the lattice sites of mobile ions in 6,955 Li-, Na-, Mg- and Al-containing ionic compounds extracted from the Inorganic Crystal Structure Database. In addition, various quantitative descriptors of the network can be used to identify and rank the materials and further used in materials databases for machine learning.
Last. Siqi Shi(SHU: Shanghai University)H-Index: 39
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The combination of a materials database with high-throughput ion-transport calculations is an effective approach to screen for promising solid electrolytes. However, automating the complicated preprocessing involved in currently widely used ion-transport characterization algorithms, such as the first-principles nudged elastic band (FP-NEB) method, remains challenging. Here, we report on high-throughput screening platform for solid electrolytes (SPSE) that integrates a materials database with hie...
Last. Siqi Shi(SHU: Shanghai University)H-Index: 39
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Abstract Inorganic solid electrolytes have obvious advantages on safety and electrochemical stability compared to organic liquid electrolytes, but the advance on high ionic conductivity of typical electrolytes is still undergoing. Although the first-principles calculation in the ion migration simulation is an important strategy to develop high-performance solid electrolyte, the process is very time-consuming. Here, we propose an effective method by combining the geometrical analysis and bond val...
Molecular dynamics is a versatile and powerful method to study diffusion in solid-state ionic conductors, requiring minimal prior knowledge of equilibrium or transition states of the system's free energy surface. However, the analysis of trajectories for relevant but rare events, such as a jump of the diffusing mobile ion, is still rather cumbersome, requiring prior knowledge of the diffusive process in order to get meaningful results. In this work we present a novel approach to detect the relev...
Last. Lin-Wang Wang(LBNL: Lawrence Berkeley National Laboratory)H-Index: 80
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Viewing the possible Li-ion migration pathways in solid state electrolytes and electrode materials is an important prerequisite for the development of all-solid-state battery materials. For high throughput material screening, it is important to have fast methods to determine the possible Li-ion pathways. In this study, by combining the traditional bond valence (BV) method with the Ewald summation method, a new BV-Ewald method was developed to calculate the Li ion diffusion map. The advantage of ...
Abstract The geometrical-topological approach based on the Voronoi partition theory has been applied in a high-throughput search for new potential potassium solid electrolytes. After screening the Inorganic Crystal Structure Database (release 2017/2), we have selected 374 ternary and quaternary potassium- and oxygen-containing compounds possessing one-, two- or three-periodic K+-ion migration maps (143, 92, and 139 compounds, respectively). Out of them, 280 compounds have not been mentioned in t...
#1Xingfeng He(UMD: University of Maryland, College Park)H-Index: 14
#2Yizhou Zhu(UMD: University of Maryland, College Park)H-Index: 17
Last. Yifei Mo(UMD: University of Maryland, College Park)H-Index: 39
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Ab initio molecular dynamics (AIMD) simulation is widely employed in studying diffusion mechanisms and in quantifying diffusional properties of materials. However, AIMD simulations are often limited to a few hundred atoms and a short, sub-nanosecond physical timescale, which leads to models that include only a limited number of diffusion events. As a result, the diffusional properties obtained from AIMD simulations are often plagued by poor statistics. In this paper, we re-examine the process to...
AbstractIncreasing attention has been paid to materials informatics approaches that promise efficient and fast discovery and optimization of functional inorganic materials. Technical breakthrough is urgently requested to advance this field and efforts have been made in the development of materials descriptors to encode or represent characteristics of crystalline solids, such as chemical composition, crystal structure, electronic structure, etc. We propose a general representation scheme for crys...
Abstract In this work, we present a combined approach comprising of crystallochemical methods such as Voronoi-Dirichlet partition (VDP), bond valence sums mapping (BVSM) and bond valence energy landscapes (BVEL) for the search for Na-ion cathode materials. Using this approach a systematic screening of the inorganic crystal structure database (ICSD-2016/2) was performed to extract potential cathode materials for Na-ion batteries. As a result, a down-selected and reviewed list of known and newly d...
Abstract Compared with conventional lithium-ion batteries, all-solid-state lithium batteries (ASSLBs) based on inorganic solid electrolytes (ISEs) are relatively new research hotspots, which can overcome tough challenges in conventional lithium-ion batteries, such as potential combustion accidents resulted from flammable liquid electrolyte solvent, low energy density, and fussy manufacturing process. In this review, we focus on the ionic conductivity and stability of ISEs by discussing defect ch...
Abstract null null Identifying descriptors linked to Li+ conduction enables rational design of solid state electrolytes (SSEs) for advanced lithium ion batteries, but it is hindered by the diverse and confounding descriptors. To address this, by integrating global and local effects of Li+ conduction environment, we develop a generic method of hierarchically encoding crystal structure (HECS) and inferring causality to identify descriptors for Li+ conduction in SSEs. Taking the cubic Li-argyrodite...
Last. John W. Lawson(ARC: Ames Research Center)H-Index: 17
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All-solid-state batteries with Li metal anode can address the safety issues surrounding traditional Li-ion batteries as well as the demand for higher energy densities. However, the development of solid electrolytes and protective anode coatings possessing high ionic conductivity and good stability with Li metal has proven to be a challenge. Here, we present our informatics approach to explore the Li compound space for promising electrolytes and anode coatings using high-throughput multi-property...
Stable and fast ionic conductors for magnesium cathode materials have the prospect of enabling high energy density batteries beyond current Lithium-ion technologies. So far, only a few candidate materials have been identified leading to data only being scarcely available to the community. Here, we present a systematic study, in the framework of Density Functional Theory, including the estimation of the diffusion barrier for 16 materials through employing Nudged Elastic Band (NEB) calculations. B...
Antiperovskites exhibit promising potential in the application of all-solid-state batteries due to their high ionic conductivity. A comprehensive understanding of the diffusion mechanism of alkali ions in antiperovskites is significant to explore novel antiperovskite electrolyte materials. In this work, we report the migration mechanism of alkali ions in Ruddlesden–Popper (RP) antiperovskites A4OX2 (A = Li, Na; X = Cl, Br, I) through first-principles calculations. Migration mechanisms of differe...
Last. Siqi Shi(SHU: Shanghai University)H-Index: 39
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Abstract High-throughput analysis of the ion transport pathways is critical for screening fast ion conductors. Currently, empirical methods, such as the geometric analysis and bond valence site energy (BVSE) methods, are respectively used for the task. Geometric analysis method can only extract geometric and topological pathway properties without considering the interatomic interactions, while the BVSE method alone does not yield a geometric classification of the sites and interstices forming th...
#1Hillary Pan(LBNL: Lawrence Berkeley National Laboratory)H-Index: 1
#2Alex M. Ganose(LBNL: Lawrence Berkeley National Laboratory)H-Index: 20
Last. Anubhav Jain(LBNL: Lawrence Berkeley National Laboratory)H-Index: 1
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Coordination numbers and geometries form a theoretical framework for understanding and predicting materials properties. Algorithms to determine coordination numbers automatically are increasingly used for machine learning (ML) and automatic structural analysis. In this work, we introduce MaterialsCoord, a benchmark suite containing 56 experimentally derived crystal structures (spanning elements, binaries, and ternary compounds) and their corresponding coordination environments as described in th...