[en] This paper reviews the rapid progress in the field of high-throughput modeling based on the Materials Genome Initiative, and its application in the discovery and design of lithium battery materials. It offers examples of screening, optimization and design of electrodes, electrolytes, coatings, additives, etc. and the possibility of introducing the machine learning method into material design. The application of the material genome method in the development of lithium battery materials provides the possibility to speed up the upgrading of new candidates in the discovery of lots of functional materials. (topical review)

[en] Discovery of a new superconductor with distinct crystal structure and chemistry often provides great opportunity for further expanding superconductor material base, and also leads to better understanding of superconductivity mechanisms. Here, we report the discovery of superconductivity in a new intermetallic oxide Hf₃Pt₄Ge₂O synthesized through a solid-state reaction. The Hf₃Pt₄Ge₂O crystallizes in a cubic structure (space group Fm-3m) with a lattice constant of a = 1.241 nm, whose stoichiometry and atomic structure are determined by electron microscopy and x-ray diffraction techniques. The superconductivity at 4.1 K and type-II superconducting nature are evidenced by the electrical resistivity, magnetic susceptibility, and specific heat measurements. The intermetallic oxide Hf₃Pt₄Ge₂O system demonstrates an intriguing structural feature that foreign oxygen atoms can be accommodated in the interstitial sites of the ternary intermetallic framework. We also successfully synthesized a series of Hf₃Pt₄Ge₂O_{1 + δ} (–0.25 ≤ δ ≤ 0.5), and found the δ-dependent superconducting transition temperature T _c. The atomic structure and the electronic structure are also substantiated by first-principles calculations. Our results present an entirely new family of superconductors with distinct structural and chemical characteristics, and could attract research interest in further finding new superconductors and exploring novel physics pertaining to the 5d-electron in these intermetallic compound systems. (paper)

[en] Porous hard carbons are known for their high specific capacities in lithium (Li) and sodium (Na) storage. Due to lack of layered graphitic structure but abundance of pores and high specific surface areas, the hard carbons are believed to mainly adsorb the Li and Na atoms on the surfaces of their pores rather than store them between the graphene layers. Various models have been proposed and the density functional theory (DFT) calculations have been carried out, but the mechanism of Li and Na storage in these materials is still unclear due to the complicated structure of the hard carbons. In this article, the Li and Na storage is simulated by considering various configurations of Li and Na atom adsorption on pure graphene edges. It shows that, with increasing number of the adsorbed atoms, the Li and Na atoms are firstly strongly adsorbed on the edges and then adsorbed near the edges. Finally, they become condensed on the edges and form a quasi-metal or metal. These findings help to understand the mechanisms of Li and Na adsorption in the hard carbons, to guide the structural design of porous hard carbons and to improve their Li and Na storage performances.

[en] Based upon advances in theoretical algorithms, modeling and simulations, and computer technologies, the rational design of materials, cells, devices, and packs in the field of lithium-ion batteries is being realized incrementally and will at some point trigger a paradigm revolution by combining calculations and experiments linked by a big shared database, enabling accelerated development of the whole industrial chain. Theory and multi-scale modeling and simulation, as supplements to experimental efforts, can help greatly to close some of the current experimental and technological gaps, as well as predict path-independent properties and help to fundamentally understand path-independent performance in multiple spatial and temporal scales. (topical review)

[en] An incompressible Co₅₄Ta₁₁B₃₅ bulk metallic glass (BMG) was investigated using in situ high-pressure synchrotron diffraction and nanoindendation. The elastic constants were deduced from the experiments based on the isotropic model. The Vickers hardness was measured to be 17.1 GPa. The elastic moduli and hardness are the highest values known in BMGs. The theoretically calculated elastic properties by density-functional study were well consistent with experimental measurements. The analysis of charge density and bonding character indicates the covalent character of Co-B and B-B bonds, underlying the unusually high elastic modulus and hardness in this material.

[en] Highlights: • Vacancy assisted and interstitial Li/Na ion diffusion mechanisms are elucidated. • The bottlenecks that determine one-step Li diffusion are come up in NASICON phase. • Comprehensive picture of fast ionic conducting mechanism is therefore proposed to account for the experimental results. The electrochemical property of solid electrolyte plays a key role in stabilizing and enhancing the performance of all solid Li-ion battery, which means numerous effort is necessitated to explore and design better solid electrolytes. In this context, density functional theory calculations (DFT) were employed to investigate the electronic structures and ionic transport properties of NASICON MTi₂(PO₄)₃ (M = Li, Na) materials aiming to elucidate the fast-ionic conductivity mechanism. The calculation results demonstrated that during the M ion migration, the Li/Na ions exhibit in both vacancy assisted and interstitial hopping, while the interstitial Li/Na diffusion with activation energies of 0.25 eV for Li and 0.49 eV for Na, is the kinetically favorable transport mechanism in their thermo-dynamically equilibrated configurations. However, the appearance of the interstitial M ion is strongly related to the ionic defect states and temperature, which indicates in real condition, two kinds of diffusion mechanism exhibit synergistic effect on the ion transport to realize the fast ion conducting in MTi₂(PO₄)₃ (M = Li, Na) materials.

[en] A family of Mn-rich bulk metallic glasses (BMGs) was developed through the similar solvent elements (SSE) substitution of Mn for Fe in (Mn_xFe_8_0_−_x)P_1_0B_7C_3 alloys. The effect of the SSE substitution on glass formation, thermal stability, elastic constants, mechanical properties, fracture morphologies, Weibull modulus and indentation fracture toughness was discussed. A thermodynamics analysis provided by Battezzati et al. (L. Battezzati, E. Garrone, Z. Metallkd. 75 (1984) 305–310) was adopted to explain the compositional dependence of the glass-forming ability (GFA). The elastic moduli follow roughly linear correlations with the substitution concentration of Mn in (Mn_xFe_8_0_−_x)P_1_0B_7C_3 BMGs. The introduction of Mn to replace Fe significantly decreases the plasticity of the resulting BMGs and the Weibull modulus of the fracture strength. A super-brittle Mn-based BMGs of (Mn_5_5Fe_2_5)P_1_0B_7C_3 BMGs were found with the indentation fracture toughness (K_c) of 1.91±0.04 MPa m"1"/"2, the lowest value among all kinds of BMGs so far. The atomic and electronic structure of the selected BMGs were simulated by the first principles molecular dynamics calculations based on density functional theory, which provided a possible understanding of the brittleness caused by the similar chemical element replacement of Mn for Fe

[en] Highlights: • The coated Li2SiO3 contributes to the cycling stability ofLMNCO. • The formation of surface solid solution could facilitate the Li diffusion kinetics. • The underlying surface/interface reaction mechanism on LMNCO is revealed. - Abstract: With the desirable energy densities, Li-rich layered cathodes have attracted great attention as potential candidates for next generation Li-ion batteries (LIBs). In this context, the Li-rich layered cathode Li[Li_0.2Mn_0.56Ni_0.17Co_0.07]O₂ (LMNCO) is prepared and surface modified homogeneously with Li-conductive Li₂SiO₃ layer via a facile co-precipitation process. It is found that the 3 wt% Li₂SiO₃ modified Li-rich cathode delivers a specific capacity as high as 207 mAh g⁻¹ after 50 cycles, which results from the interplay among the electrode, Li₂SiO₃ coating layer and the electrolyte. Further analysis indicates that the Li₂SiO₃ layer could effectively balance the exfoliation of surface alkaline speciation and the dissolution of surface transition metal to generate the LiMnNiCoSiO protection layer, which will beneficial to the Li surface diffusion kinetics and the electrochemical stability of Li-rich layered materials as well.

[en] All solid-state battery (ASSB) is widely recognized as one of the most promising high-energy-density systems/technologies. However, thermal safety issues induced by highly reactive materials still exist for solid electrolytes (SEs). Insights on thermal behaviors at elevated temperatures and the underlying mechanism for thermal stability of SE-based systems are still missing. Herein, thermal stability performance of typical sulfide SEs is systematically investigated with metal Li, whose order of interfacial thermal stability is concluded to be Li${}_6$PS${}_5$Cl > Li${}_3$PS${}_4$ > Li${}_{9.54}$Si${}_{1.74}$P${}_{1.44}$S${}_{11.7}$Cl${}_{0.3}$ > Li${}_4$SnS${}_4$ > Li${}_7$P${}_3$S${}_{11}$ after a comprehensive evaluation. Interestingly, Li${}_4$SnS${}_4$, which achieves good air stability, has poor thermal stability with Li metal. This is possibly caused by Li-Sn alloy products generated during thermal decomposition, and their great thermodynamic driving force towards SE for accelerated thermal runaway. Moreover, electrolytes with poor material-level thermal stability (e.g., Li${}_7$P${}_3$S${}_{11}$) may form a dense passivation layer by self-decomposition with Li metal to retard thermal runaway. Conclusively, the material structure affects the thermodynamic stability of the system, but the reaction products (interphase) affects the kinetic process of the thermal reaction within a certain temperature range. Therefore, thermal stability with both metallic lithium and decomposition products is a necessary condition for interfacial thermal stability of sulfide SEs. (© 2023 Wiley‐VCH GmbH)