Encapsulating atomic molybdenum into hierarchical nitrogen-doped carbon nanoboxes for efficient oxygen reduction.

Construction of single-atom catalysts (SACs) with maximally exposed active sites remains a challenging task mainly because of the lack of suitable host matrices. In this study, hierarchical N-doped carbon nanoboxes composed of ultrathin nanosheets with dispersed atomic Mo (denoted as hierarchical SA-Mo-C nanoboxes) were fabricated via a template-engaged multistep synthesis process. Comprehensive characterizations, including X-ray absorption fine structure analysis, reveal the formation of Mo-N4 atomic sites uniformly anchored on the hierarchical carbon nanoboxes. The prepared catalysts offer structural and morphological advantages, including ultrathin nanosheet units, unique hollow structures and abundant active Mo-N4 species, that result in excellent activity with a half-wave potential of 0.86 V vs. RHE and superb stability for the oxygen reduction reaction in 0.1 M KOH; thus, the catalysts are promising air-cathode catalysts for Zn-air batteries with a high peak power density of 157.6 mW cm-2.

Facile Surfactant-, Reductant-, and Ag Salt-free Growth of Ag Nanoparticles with Controllable Size from 35 to 660 nm on Bulk Ag Materials.

Morphologically and dimensionally controlled growth of Ag nanocrystals has long been plagued by surfactants or capping agents that complicate downstream applications, unstable Ag salts that impaired the reproducibility, and multistep seed injection that is troublesome and time-consuming. Here, we report a one-pot electro-chemical method to fast (∼2 min) produce Ag nanoparticles from commercial bulk Ag materials in a nitric acid solution, eliminating any need for surfactants or capping agents. Their size can be easily manipulated in an unprecedentedly wide range from 35 to 660 nm. Furthermore, the Ag nanoparticles are directly grown on the Ag substrate, highly desirable for promising applications such as catalysis and plasmonics. The mechanistic studies reveal that the concentration of Ag+ in the diffusion layer nearby the surface, controlled by the magnitude and duration of voltage, is critical in governing the nanoparticle formation (<1.3 mM) and its dimensional adjustability.

In situ tensile fracturing of multilayer graphene nanosheets for their in-plane mechanical properties.

The excellent mechanical properties of single- and few-layer graphene have been well-quantified and evidenced by computational methods and local indentation measurements. However, there are less experimental reports on the in-plane mechanical properties of multilayer graphene sheets, despite many practical applications in flexible electronic and energy devices (e.g. graphene flexible electronic display, battery, and storage devices) are actually based on these thicker nanosheets. Here, in-plane fracture behaviors of multilayer graphene nanosheets with thicknesses between ∼10 and 300 nm (∼10-1000 layers) are characterized and quantified by in situ scanning electron microscopy and transmission electron microscopy under tensile loading. We found that, generally, the fracture strengths of graphene nanosheets decrease as the thickness (or layers) increases; however, the fracture strain of thinner graphene sheets is less than that of thicker sheets. The fracture process of the thicker nanosheets includes the initial flattened stage, the stable elastic stage, and the rapid fracture with brittle characteristics, while the thinner nanosheets show obvious delamination between the atomic layers at fracture. This work provides critical experimental insights into the tensile fracture behavior of multilayer two-dimensional materials and a better understanding on their realistic mechanical performance for potential flexible device and composite applications.

Large-scale synthesis of carbon dots/TiO2 nanocomposites for the photocatalytic color switching system.

In view of the easy control and contactless spatial nature of light, the photoreversible color switching system has attracted tremendous attention. Although some progress has been achieved in the past few years, the practical applications have been limited by the complicated preparation process, material toxicity and low reaction yield. Herein, we report a rapid, a one-pot large-scale synthesis approach for the preparation of carbon dots (CDs)/TiO2 nanocomposites via the thermal condensation at 160 °C, affording high photocatalytic color switching on/off performance. Under ambient conditions and with the introduction of some oxygen gas, MB rapidly changed from blue to colorless in one minute under UV-vis irradiation and recovered (again showed its original blue color) in twenty minutes. We anticipate that the designed low-cost and green carbon dots (CDs)/TiO2 nanocomposites have much potential in practical applications and represent a solid step toward color switching applications.

Multicolor Tuning and Temperature-Triggered Anomalous Eu3+-Related Photoemission Enhancement via Interplay of Accelerated Energy Transfer and Release of Defect-Trapped Electrons in the Tb3+,Eu3+-Doped Strontium-Aluminum Chlorites.

So far, a large number of rare earth (RE) and non-RE-doped emission-tunable crystals based on controllable energy transfer have become available, but numerous mechanistic issues, particularly for those that involve temperature-dependent energy transfer between the well-shielded 4f RE ions, lack comprehensive theoretical and experimental investigation, limiting greatly their development and applications in the future. Here, we design and report a type of Tb3+,Eu3+-doped Sr3Al2O5Cl2 phosphors capable of multiemissions upon excitation at 376 nm, through using the orthorhombic Sr3Al2O5Cl2 as the host lattice while the well-shielded 4f Tb3+ and Eu3+ ions as dual luminescent centers. Our results reveal that the energy transfer from Tb3+ to Eu3+ ions, happening via an electric dipole-quadrupole (d-q) interaction, can be controlled by the doping ratio of Tb3+ and Eu3+, leading to the tunable emissions from green (0.3159, 0.5572) to red (0.6579, 0.3046). It is found from time-resolved photoluminescence (PL) spectra that this energy transfer begins at t = 5 µs and gradually ends at t ≥ 200 µs. Moreover, from temperature-dependent PL results, we reveal that the Eu3+ emission features an anomalous intensity enhancement at the earlier heating state. With the density functional theory (DFT) calculations, we have screened the possibilities of site preferential substitution problem. By jointly taking into account the X-ray diffraction Rietveld refinement, DFT findings, and PL and thermoluminescence spectra, a mechanistic profile is proposed for illustrating the PL observations. In particular, our discussions reveal that the temperature-triggered Eu3+ emission enhancement is due to the interplay of the temperature-induced accelerated energy transfer and defect-trapped electrons that are released upon the thermal stimulation. Unlike most of reported phosphor materials that are always suggested for phosphor-converted white light-emitting diodes, we propose new application possibilities for Tb3+,Eu3+-doped Sr3Al2O5Cl2 phosphors, such as anticounterfeiting, temperature-controlled fluorescence sensor, data storage, and security devices.