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.

Sonodynamic therapy (SDT) can overcome the critical issue of depth-penetration barrier of photo-triggered therapeutic modalities. However, the discovery of sonosensitizers with high sonosensitization efficacy and good stability is still a significant challenge. In this study, the great potential of a metal-organic-framework (MOF)-derived carbon nanostructure that contains porphyrin-like metal centers (PMCS) to act as an excellent sonosensitizer is identified. Excitingly, the superior sonosensitization effect of PMCS is believed to be closely linked to the porphyrin-like macrocycle in MOF-derived nanostructure in comparison to amorphous carbon nanospheres, due to their large highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) gap for high reactive oxygen species (ROS) production. The nanoparticle-assisted cavitation process, including the visualized formation of the cavitation bubbles and microjets, is also first captured by high-speed camera. High ROS production in PMCS under ultrasound is validated by electron spin resonance and dye measurement, followed by cellular destruction and high tumor inhibition efficiency (85%). This knowledge is important from the perspective of understanding the structure-dependent SDT enhancement of a MOF-derived carbon nanostructure.

Nanozymes have attracted extensive interest owing to their high stability, low cost and easy preparation, especially in the field of cancer therapy. However, the relatively low catalytic activity of nanozymes in the tumor microenvironment (TME) has limited their applications. Herein, we report a novel nanozyme (PtFe@Fe3O4) with dual enzyme‐like activities for highly efficient tumor catalytic therapy. PtFe@Fe3O4 shows the intrinsic photothermal effect as well as photo‐enhanced peroxidase‐like and catalase‐like activities in the acidic TME, thereby effectively killing tumor cells and overcoming the tumor hypoxia. Importantly, a possible photo‐enhanced synergistic catalytic mechanism of PtFe@Fe3O4 was first disclosed. We believe that this work will advance the development of nanozymes in tumor catalytic therapy.

Atomically dispersed metal catalysts (ADCs), as an emerging class of heterogeneous catalysts, have been widely investigated during the past two decades. The atomic dispersion nature of the catalytic metal centers makes them an ideal system for bridging homogeneous and heterogeneous metal catalysts. The recent rapid development of new synthetic strategies has led to the explosive growth of ADCs with a wide spectrum of metal atoms dispersed on supports of different chemical compositions and natures. The availability of diverse ADCs creates a powerful materials platform for investigating mechanisms of complicated heterogeneous catalysis at the atomic levels. Considering most dispersed metal atoms on ADCs are coordinated by the donors from supports, this review will demonstrate how the surface coordination chemistry plays an important role in determining the catalytic performance of ADCs. This review will start from the link between coordination chemistry and heterogeneous catalysis. After the brief description on the advantages and limitations of common structure characterization methods in determining the coordination structure of ADCs, the surface coordination chemistry of ADCs on different types of supports will be discussed. We will mainly illustrate how the local and vicinal coordination species on different support systems act together with the dispersed catalytic metal center to determine the catalytic activity, selectivity, and stability of ADCs. The dynamic coordination structure change of ADCs in catalysis will be highlighted. At the end of the review, personal perspectives on the further development of the field of ADCs will be provided.

The improved ionic conductivity (1.64 × 10(-4) S cm(-1) at room temperature) and excellent electrochemical stability of nanoporous β-Li3PS4 make it one of the promising candidates for rechargeable all-solid-state lithium-ion battery electrolytes. Here, elastic properties, defect thermodynamics, phase diagram, and Li(+) migration mechanism of Li3PS4 (both γ and β phases) are examined via the first-principles calculations. Results indicate that both γ- and β-Li3PS4 phases are ductile while γ-Li3PS4 is harder under volume change and shear stress than β-Li3PS4. The electrochemical window of Li3PS4 ranges from 0.6 to 3.7 V, and thus the experimentally excellent stability (>5 V) is proposed due to the passivation phenomenon. The dominant diffusion carrier type in Li3PS4 is identified over its electrochemical window. In γ-Li3PS4 the direct-hopping of Lii(+) along the [001] is energetically more favorable than other diffusion processes, whereas in β-Li3PS4 the knock-off diffusion of Lii(+) along the [010] has the lowest migration barrier. The ionic conductivity is evaluated from the concentration and the mobility calculations using the Nernst-Einstein relationship and compared with the available experimental results. According to our calculated results, the Li(+) prefers to transport along the [010] direction. It is suggested that the enhanced ionic conductivity in nanostructured β-Li3PS4 is due to the larger possibility of contiguous (010) planes provided by larger nanoporous β-Li3PS4 particles. By a series of motivated and closely linked calculations, we try to provide a portable method, by which researchers could gain insights into the physicochemical properties of solid electrolyte.

Background Mangroves are ecologically and economically important forests of the tropics. As one of the most carbon-rich biomes, mangroves account for 11% of the total input of terrestrial carbon into oceans. Although viruses are considered to significantly influence local and global biogeochemical cycles, little information is available regarding the community structure, genetic diversity and ecological roles of viruses in mangrove ecosystems. Methods Here, we utilised viral metagenomics sequencing and virome-specific bioinformatics tools to study viral communities in six mangrove soil samples collected from different mangrove habitats in Southern China. Results Mangrove soil viruses were found to be largely uncharacterised. Phylogenetic analyses of the major viral groups demonstrated extensive diversity and previously unknown viral clades and suggested that global mangrove viral communities possibly comprise evolutionarily close genotypes. Comparative analysis of viral genotypes revealed that mangrove soil viromes are mainly affected by marine waters, with less influence coming from freshwaters. Notably, we identified abundant auxiliary carbohydrate-active enzyme (CAZyme) genes from mangrove viruses, most of which participate in biolysis of complex polysaccharides, which are abundant in mangrove soils and organism debris. Host prediction results showed that viral CAZyme genes are diverse and probably widespread in mangrove soil phages infecting diverse bacteria of different phyla. Conclusions Our results showed that mangrove viruses are diverse and probably directly manipulate carbon cycling by participating in biomass recycling of complex polysaccharides, providing the knowledge essential in revealing the ecological roles of viruses in mangrove ecosystems. Electronic supplementary material The online version of this article (10.1186/s40168-019-0675-9) contains supplementary material, which is available to authorized users.

Deciphering the molecular pictures of the multi‐component and non‐periodic organic‐inorganic interlayer is a grand technical challenge. Here we show that the atomic arrangement of hybrid surface ligands on metal nanoparticles can be precisely quantified through comprehensive characterization of a novel gold cluster, Au44(iPr2‐bimy)9(PA)6Br8 (1), which features three types of ligands, namely, carbene (1,3‐diisopropylbenzimidazolin‐2‐ylidene, iPr2‐bimy), alkynyl (phenylacetylide, PA), and halide (Br), respectively. The delicately balanced stereochemical effects and bonding capabilities of the three ligands give rise to peculiar geometrical and electronic structures. Remarkably, despite its complex and highly distorted surface structure, cluster 1 exhibits unusual catalytic properties and yet it is highly stable, both chemically and thermally. Moreover, rich reactive sites on the cluster surface raise the prospect of bio‐compatibility (as it can be functionalized to yield water‐soluble derivatives) and bio‐applications.

The complexity of heterogeneous metal catalysts makes it challenging to gain insights into their catalytic mechanisms. Thus, there exists a huge gap between heterogeneous catalysis and organometallic catalysis. With the success in the preparation of highly robust atomically precise metal nanocluster catalysts (i.e., [Au16(NHC-1)5(PA)3Br2]3+ and [Au17(NHC-1)4(PA)4Br4]+, where NHC-1 is a bidentate NHC ligand, and PA is phenylacetylide) with surface organometallic motifs anchored on the metallic core, we demonstrate in this work how the metallic core works synergistically with the surface organometallic motifs to enhance the catalysis. More importantly, the discovery allows the development of highly stable and recyclable heterogeneous metal catalysts to achieve efficient hydroamination of alkynes with an extremely low catalyst dosage (0.002 mol %), helping bridge the gap between heterogeneous and homogeneous metal catalysis. The surface modification of metal nanocatalysts with organometallic motifs provides a new design principle of metal catalysts with enhanced catalysis.