Lithium-sulphur batteries are one very appealing power source with high energy density. But their practical use is still hindered by several issues including short lifespan, low efficiency and safety concern from the lithium anode. Polysulphide dissolution and insulating nature of sulphur are generally considered responsible for the capacity degradation. However, the detachment of discharge products, that is, highly polar lithium sulphides, from nonpolar carbon matrix (for example, graphene) has been rarely studied as one critical factor. Here we report the strongly covalent stabilization of sulphur and its discharge products on aminofunctionalized reduced graphene oxide that enables stable capacity retention of 80% for 350 cycles with high capacities and excellent high-rate response up to 4 C. The present study demonstrates a feasible and effective strategy to solve the long-term cycling difficulty for lithium-sulphur batteries and also helps to understand the capacity decay mechanism involved.

The integrated hybrid architectures composed of edge site-enriched nickel–cobalt sulfide (Ni–Co–S) nanoparticles and graphene as advanced materials for asymmetric supercapacitors are configured, delivering a superb rate capability.

Inside a liquid solution, oriented attachment (OA) is now recognized to be as important a pathway to crystal growth as other, more conventional growth mechanisms. However, the driving force that controls the occurrence of OA is still poorly understood. Here, using in-situ liquid cell transmission electron microscopy, we demonstrate the ligand-controlled OA of citrate-stabilized gold nanoparticles at atomic resolution. Our data reveal that particle pairs rotate randomly at a separation distance greater than twice the layer thickness of adsorbed ligands. In contrast, when the particles get closer, their ligands overlap and guide the rotation into a directional mode until they share a common {111} orientation, when a sudden contact occurs accompanied by the simultaneous expulsion of the ligands on this surface. First-principle calculations confirm that the lower ligand binding energy on {111} surfaces is the intrinsic reason for the preferential attachment at this facet, rather than on other low-index facets.

Single‐atom catalysts (SACs) with individual and isolated metal atoms anchored to supports can act as active centers. Single‐atom catalysis is powerful and attractive because SACs have demonstrated distinguishing performances, such as drastic cost‐reduction, notable catalytic activity, and selectivity. Herein, we firstly introduce SAC, including the concept and some key issues in synthesis and catalysis. Then, the power of single‐atom catalysis is highlighted and the most recent advances are summarized. It is very encouraging that in recent years our understanding of SACs has increased, owing to substantial studies regarding sample preparation, characterization, evaluation, and also mechanistic interpretation. On the other hand, great challenges still remain for SACs.

Using porous materials to cope with environmental issues is promising but remains a challenge especially for removing the radioactive vapor wastes in fission because of harsh adsorption conditions. Here we report a new, stable covalent organic framework (COF) as a porous platform for removing iodine vapor-a major radioactive fission waste. The three-dimensional COF consists of a diamond topology knotted by adamantane units, creates ordered one-dimensional pores and are highly porous. The COF enables the removal of iodine vapor via charge transfer complex formation with the pore walls to achieve exceptional capacity. Moreover, the 3D COF is "soft" to trigger structural fitting to iodine while retaining connectivity and enables cycle use for many times while retaining high uptake capacity. These results set a new benchmark for fission waste removal and suggest the great potential of COFs as a designable porous material for challenging world-threatening pollution issues.

BackgroundHydroxylated polybrominated diphenyl ethers (HO-PBDEs) may disrupt thyroid hormone status because of their structural similarity to thyroid hormone. However, the molecular mechanisms of interactions with thyroid hormone receptors (TRs) are not fully understood.ObjectivesWe investigated the interactions between HO-PBDEs and TRβ to identify critical structural features and physicochemical properties of HO-PBDEs related to their hormone activity, and to develop quantitative structure–activity relationship (QSAR) models for the thyroid hormone activity of HO-PBDEs.MethodsWe used the recombinant two-hybrid yeast assay to determine the hormone activities to TRβ and molecular docking to model the ligand–receptor interaction in the binding site. Based on the mechanism of action, molecular structural descriptors were computed, selected, and employed to characterize the interactions, and finally a QSAR model was constructed. The applicability domain (AD) of the model was assessed by Williams plot.ResultsThe 18 HO-PBDEs tested exhibited significantly higher thyroid hormone activities than did PBDEs (p < 0.05). Hydrogen bonding was the characteristic interaction between HO-PBDE molecules and TRβ, and aromaticity had a negative effect on the thyroid hormone activity of HO-PBDEs. The developed QSAR model had good robustness, predictive ability, and mechanism interpretability.ConclusionsHydrogen bonding and electrostatic interactions between HO-PBDEs and TRβ are important factors governing thyroid hormone activities. The HO-PBDEs with higher ability to accept electrons tend to have weak hydrogen bonding with TRβ and lower thyroid hormone activities.

In order to overcome the shuttling effect of soluble polysulfides in lithium–sulfur (Li–S) batteries, we have designed and synthesized a creative MoS2–MoO3/carbon shell (MoS2–MoO3/CS) composite by a H2O2-enabled oxidizing process under mild conditions, which is further used for separator modification. The MoS2–MoO3 heterostructures can conform to the CS morphology, forming two-dimensional nanosheets, and thus shorten the transport path of lithium ion and electrons. Based on our theoretical calculations and experiments, the heterostructures show strong surface affinity toward polysulfides and good catalytic activity to accelerate polysulfide conversion. Benefiting from the above merits, the Li–S battery with a MoS2–MoO3/CS modified separator exhibits good electrochemical performance: it delivers a high discharge capacity of 1531 mAh g–1 at 0.2 C; the initial capacity can be maintained by 92% after 600 cycles at 1 C, and the discharge capacity decay rate is only 0.0135% per cycle. Moreover, the MoS2–MoO3/CS battery still achieves good cycling stability with 78% capacity retention after 100 cycles at 0.2 C with a high sulfur loading of 5.9 mg cm–2. This work offers a facile design to construct the MoS2–MoO3 heterostructures for high-performance Li–S batteries, and may also improve one’s understanding on the heterostructure contribution during polysulfide adsorption and conversion.

Superior electrocatalytic activities and excellent electrochemical stabilities of inexpensive counter electrodes (CEs) are crucial to the large‐scale practical application of dye‐sensitized solar cells (DSSCs). Herein, an efficient strategy for fabricating nitrogen‐doped graphene nanoribbons (N‐GNRs) via chemical unzipping of carbon nanotubes coupled with nitrogen doping process is reported, where abundant edge sites are produced and fully exposed basal planes of GNRs are activated by the N atoms within GNRs backbone. Benefiting from such unique characteristics, when first applied as CEs for DSSCs with triiodide/iodide electrolyte, a power conversion efficiency of 8.57% is delivered, outperforming GNRs (8.01%) and being superb to that of Pt (7.84%), and outstanding electrochemical stabilities of N‐GNRs are also demonstrated. Density functional theory calculations reveal that the N species within GNRs matrix, especially the predominant quaternary ones, could remarkably decrease the ionization energy of GNRs, which is instrumental to transfer electrons rapidly from external circuit to triiodide, and reduce charge‐transfer resistance, thus contributing to the enhanced photovoltaic performance. The present work has an insight into the unique role of N species on GNRs to the triiodide reduction, and provides an efficient strategy for design of high‐efficiency carbon electrodes with fully exposed active sites in energy conversion/storage devices.