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Recently emerging lithium ternary chlorides have attracted increasing attention for solid‐state electrolytes (SSEs) due to their favorable combination between ionic conductivity and electrochemical stability. However, a noticeable discrepancy in Li‐ion conductivity persists between chloride SSEs and organic liquid electrolytes, underscoring the need for designing novel chloride SSEs with enhanced Li‐ion conductivity. Herein, an intriguing trigonal structure (i.e., Li3SmCl6 with space group P3112) is identified using the global structure searching method in conjunction with first‐principles calculations, and its potential for SSEs is systematically evaluated. Importantly, the structure of Li3SmCl6 exhibits a high ionic conductivity of 15.46 mS cm−1 at room temperature due to the 3D lithium percolation framework distinct from previous proposals, associated with the unique in‐plane cation ordering and stacking sequences. Furthermore, it is unveiled that Li3SmCl6 possesses a wide electrochemical window of 0.73−4.30 V vs Li+/Li and excellent chemical interface stability with high‐voltage cathodes. Several other Li3MCl6 (M = Er, and In) materials with isomorphic structures to Li3SmCl6 are also found to be potential chloride SSEs, suggesting the broader applicability of this structure. This work reveals a new class of ternary chloride SSEs and sheds light on strategy for structure searching in the design of high‐performance SSEs. [ABSTRACT FROM AUTHOR]

Abstract Recently emerging lithium ternary chlorides have attracted increasing attention for solid‐state electrolytes (SSEs) due to their favorable combination between ionic conductivity and electrochemical stability. However, a noticeable discrepancy in Li‐ion conductivity persists between chloride SSEs and organic liquid electrolytes, underscoring the need for designing novel chloride SSEs with enhanced Li‐ion conductivity. Herein, an intriguing trigonal structure (i.e., Li3SmCl6 with space group P3112) is identified using the global structure searching method in conjunction with first‐principles calculations, and its potential for SSEs is systematically evaluated. Importantly, the structure of Li3SmCl6 exhibits a high ionic conductivity of 15.46 mS cm−1 at room temperature due to the 3D lithium percolation framework distinct from previous proposals, associated with the unique in‐plane cation ordering and stacking sequences. Furthermore, it is unveiled that Li3SmCl6 possesses a wide electrochemical window of 0.73−4.30 V vs Li+/Li and excellent chemical interface stability with high‐voltage cathodes. Several other Li3MCl6 (M = Er, and In) materials with isomorphic structures to Li3SmCl6 are also found to be potential chloride SSEs, suggesting the broader applicability of this structure. This work reveals a new class of ternary chloride SSEs and sheds light on strategy for structure searching in the design of high‐performance SSEs.

Crystal structure prediction algorithms have become powerful tools for materials discovery in recent years, however, they are usually limited to relatively small systems. The main challenge is that the number of local minima grows exponentially with the system size. In this work, we proposed two crossover-mutation schemes based on graph theory to accelerate the evolutionary structure searching by automatic decomposition methods. These schemes can detect molecules or clusters inside periodic networks using quotient graphs for crystals, and the decomposition can dramatically reduce the searching space. Sufficient examples for test, including the high-pressure phases of methane, ammonia, MgAl2O4 and boron, show that these new evolution schemes can significantly improve the success rate and searching efficiency compared with the standard method in both isolated and extended systems.

Graphical abstract Abstract The atomistic structures of solid–solid interfaces are of fundamental interests for understanding physical properties of interfacial materials. However, determination of interface structures faces a substantial challenge, both experimentally and theoretically. Here, we propose an efficient method for predicting interface structures via the generalization of our in-house developed CALYPSO method for structure prediction. We devised a lattice match toolkit that allows us to automatically search for the optimal lattice-matched superlattice for construction of the interface structures. In addition, bonding constraints (e.g., constraints on interatomic distances and coordination numbers of atoms) are imposed to generate better starting interface structures by taking advantages of the known bonding environment derived from the stable bulk phases. The interface structures evolve by following interfacially confined swarm intelligence algorithm, which is known to be efficient for exploration of potential energy surface. The method was validated by correctly predicting a number of known interface structures with only given information of two parent solids. The application of the developed method leads to prediction of two unknown grain boundary (GB) structures (r-GB and p-GB) of rutile TiO 2 Σ5(2 1 0) under an O reducing atmosphere that contained Ti3+ as the result of O defects. Further calculations revealed that the intrinsic band gap of p-GB is reduced to 0.7 eV owing to substantial broadening of the Ti-3 d interfacial levels from Ti3+ centers. Our results demonstrated that introduction of grain boundaries is an effective strategy to engineer the electronic properties and thus enhance the visible-light photoactivity of TiO 2. [ABSTRACT FROM AUTHOR]

Background: Peroxide turnover and signalling are involved in many biological phenomena relevant to human diseases. Yet, all the players and mechanisms involved in peroxide perception are not known. Elucidating very remote evolutionary relationships between proteins is an approach that allows the discovery of novel protein functions. Here, we start with three human proteins, SRPX, SRPX2 and CCDC80, involved in tumor suppression and progression, which possess a conserved region of similarity. Structure and function prediction allowed the definition of P-DUDES, a phylogenetically widespread, possibly ancient protein structural domain, common to vertebrates and many bacterial species. Results: We show, using bioinformatics approaches, that the P-DUDES domain, surprisingly, adopts the thioredoxin-like (Thx-like) fold. A tentative, more detailed prediction of function is made, namely, that of a 2-Cys peroxiredoxin. Incidentally, consistent overexpression of all three human P-DUDES genes in two public glioblastoma microarray gene expression datasets was discovered. This finding is discussed in the context of the tumor suppressor role that has been ascribed to P-DUDES proteins in several studies. Majority of non-redundant P-DUDES proteins are found in marine metagenome, and among the bacterial species possessing this domain a trend for a higher proportion of aquatic species is observed. Conclusions: The new protein structural domain, now with a broad enzymatic function predicted, may become a drug target once its detailed molecular mechanism of action is understood in detail. [ABSTRACT FROM AUTHOR]