We present the stepwise computer screening results to identify solids prone to Zn2+-ion conductivity. The rapid geometrical–topological (GT) screening based on Voronoi partition was utilized as the first step for high-throughput analysis of the ICSD. We found that 334 of 782 Zn-/O-containing compounds possess one-dimensional (1D)-, two-dimensional (2D)-, or three-dimensional (3D)-periodic Zn2+-ion migration maps. Among them, 83 compounds were previously unknown as possible Zn2+-ion conductors. We applied bond valence site energy (BVSE) calculations to evaluate the migration energies for the Zn2+-ion conduction and to ensure that this migration barrier was the lowest of all ions in the respective structure. Of the 83 compounds, 27 fulfilled the condition of being solely Zn2+ conductors. For the nine most promising compounds, we used the Nudged Elastic Band (NEB) method within the density functional theory (DFT) approach to verify Zn2+-ion conductivity. This yielded the most interesting candidates (ZnM2O4, M = Fe, Cr, V; ZnP2O6) with migration energies of less than 0.7 eV/ion. Finally, we simulated ionic conductivities within the kinetic Monte Carlo approach, compared the results of different approaches, and commented on the complexity of the promising structures. We conclude with the proposal of Zn-ion all-solid-state battery variants. The list of the novel prospective Zn2+-ion conductors with characteristics was uploaded to our database batterymaterials.info.
Essential to the quality of X‐ray analysis in crystallography, such as diffractometry and spectrometry, is a stable and reproducible X‐ray source. Commonly, different optical elements are utilized to provide a dedicated X‐ray beam. The stable alignment of all these components is a prerequisite in order to reduce aberrations and to achieve high signal‐to‐noise ratios. Besides such aberrations and electronically induced variations of the X‐ray primary beam intensity, the environmental conditions are of particular importance, most prominently the barometric pressure, humidity and temperature. In a qualitative as well as quantitative study, the influence of the environmental conditions on the primary beam intensity of a sealed tube with a Cu anode and their correlations are determined. For a common setup, utilizing a scintillation counter, laboratory as well as external conditions are monitored simultaneously for 28 d. Their individual influence on the X‐ray intensity and their correlations are evaluated by statistical analysis including time lag. By this comprehensive study, experimental intensity variations of up to ΔI/I = 1.153 ± 0.001% are determined during density of air changes of Δρ/ρ = 3.7 ± 0.6%. This is interpreted in terms of air transmission variations of up to TX‐ray = 1.137 ± 0.001% for a typical X‐ray analysis setup due to ambient barometric pressure, temperature and humidity changes for natural mid‐ and long‐term variations. Significant correlations with respect to daily and weekly cycles and in particular with ambient conditions are determined. These results are used for a time‐dependent absorption correction of the measured intensity, which reduces the standard error by about 25%.
Improvement of existing batteries is a hot topic due to both the rapid spread of mobile technologies and the impetuous growth of the electric vehicle sector. The commonly used lithium-ion batteries (LIB) have a number of well-known disadvantages: flammability and high lithium price due to limited natural resources. The moderate capacity of LIBs is a further challenge for high-performance mobile devices. Theoretically, all-solid-state batteries based on high-valent working ions, such as magnesium, zinc or aluminum, can have higher volumetric capacities compared to LIBs [1]. We report the results of the high-throughput search for new solid electrolytes (SE) and cathode materials for high-valent metal-ion batteries. We focused on Mg-, Ca-, Zn-and Al-containing ternary and quaternary chalcogenides. Theoretically, S-, Se-or Tecontaining compounds should exhibit higher cation conductivities than their oxygen analogues. It can be explained by a lower degree of ionicity in chalcogenides in comparison to oxides [2]. Our study was performed by using a well-established high-throughput screening algorithm [3]. The algorithm consists of three main steps: (a) fast topological-geometrical screening; (b) bond valence site energy (BVSE) modeling for a preliminary quantitative estimation and (c) precise quantum-chemical modeling of ionic transport. All ternary and quaternary Mg, Ca, Zn and Al chalcogenides (1572 structures) were extracted from the ICSD (version 2020/1). Among them, a group of promising cation conductors with 1D-, 2D-, or 3D-migration maps was identified by using the Voronoi partitioning algorithm as implemented in the ToposPro package [4]. We obtained 72 S-, 30 Se-and 11 Te-containing high-valent ion conductors. The BVSE method was utilized for determination of migration energies of all species in the compounds, and a group of most promising compounds with migration barriers Em ≤ 0.5 eV and the difference in the migration energies with other ions ΔEm ≥ 0.5 eV was selected. This group includes, in particular, MgLu2Se4, MgHo2Se4, ZnLa3GaSe7, Al5.9SnTe9.892, Al2Be2La6S14, Al3.3Dy6S14, Al3.3La6S14 compounds. In a final step, the density functional theory (DFT) modeling was carried out for the structures with lowest Em compounds. The Nudged Elastic Band (NEB) method was used as implemented in the VASP package [5]. Figure 1 shows a good agreement of migration maps between the three applied approaches.
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