Dual-Atom P-Co-Dy Charge-Transfer Bridge on Black Phosphorus for Enhanced Photocatalytic CO2 Reduction.

The synergistic effect of rare earth single-atoms and transition metal single-atoms may enable us to achieve some unprecedented performance and characteristics. Here, Co-Dy dual-atoms on black phosphorus with a P-Co-Dy charge-transfer bridge are designed and fabricated as the active center for the CO2 photoreduction reaction. The synergistic effect of Co-Dy on the performance of black phosphorus is studied by combining X-ray absorption spectroscopy, ultrafast spectral analysis, and in situ technology with DFT calculations. The results show that the Co and Dy bimetallic active site can promote charge transfer by the charge transfer bridge from P to Dy, and then to Co, thereby improving the photocatalytic activity of black phosphorus. The performance of catalysts excited at different wavelength light indicates that the 4G11/2/2I15/2/4F9/2→6H15/2 and 4F9/2→6H13/2 emissions of Dy can be absorbed by black phosphorus to improve the utilization of sunlight. The in situ DRIFTS and density functional theory (DFT) calculations are used to investigate the CO2 photoreduction pathway. This work provides an depth insight into the mechanism of dual-atom catalysts with enhanced photocatalytic performance, which helps to design novel atomic photocatalysts with excellent activity for CO2 reduction reactions.

Controlled growth and ion intercalation mechanism of monocrystalline niobium pentoxide nanotubes for advanced rechargeable aluminum-ion batteries.

Rechargeable aluminum-ion batteries (RAIBs) have attracted increasing attention owing to their high theoretical volumetric capacity, high resource abundance, and good safety performance. However, the existing RAIB systems usually exhibit relatively low specific capacities limited by the cathode materials. In this study, we developed a one-step chemical vapor deposition method to prepare single-crystal orthogonal Nb2O5 nanotubes for serving as high-performance electrode materials for RAIBs, showing a high reversible capability of 556 mA h g-1 at 25 mA g-1 and good thermal endurability at elevated temperatures (50 °C). A combination of a series of detailed ex situ structural characterization studies verified the reversible intercalation/deintercalation of chloroaluminate anions (AlCl4-) into/from the (001) planes of monocrystalline Nb2O5 nanotubes. It also revealed that the nanoarchitecture of Nb2O5 nanotubes with thin tube walls, hollow inner space and a short ion transport distance is conducive to the rapid kinetics of the insertion/extraction process. This work provides a promising route to design high-performance electrode materials based on transition metal compounds for RAIBs via the rational modulation of their structure and morphology.

Intermetallic SnSb nanodots embedded in carbon nanotubes reinforced nanofabric electrodes with high reversibility and rate capability for flexible Li-ion batteries.

Tin (Sn) based anode materials have been regarded as promising alternatives for graphite in lithium ion batteries (LIBs) due to their high theoretical specific capacity and conductivity. However, their practical application is severely restrained by the drastic volume variation during cycling processes. Here we report the preparation of intermetallic SnSb nanodots embedded in carbon nanotube reinforced N-doped carbon nanofibers (SnSb-CNTs@NCNFs) as a free-standing and flexible anode for LIBs. In this unique structure, the SnSb nanodots are well protected by the NCNFs and exhibit greatly reduced volume change. The mechanical strength and conductivity of the nanofabric electrode are further improved by the embedded CNTs. Benefiting from these advantages, the SnSb-CNTs@NCNFs anode delivers a high reversible capacity of 815 mA h g-1 at 100 mA g-1, a high rate capability (370 mA h g-1 at 5000 mA g-1) and a long cycle life (451 mA h g-1 after 1000 cycles at 2000 mA g-1). When assembled into flexible pouch cells, the full cells based on SnSb-CNTs@NCNFs anodes also exhibit high flexibility and good lithium storage performances.

Nitrogen-Doped Carbon Nanotube Forests Planted on Cobalt Nanoflowers as Polysulfide Mediator for Ultralow Self-Discharge and High Areal-Capacity Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries with high theoretical energy density have caught enormous attention for electrochemical power source applications. However, the development of Li-S batteries is hindered by the electrochemical performance decay that resulted from low electrical conductivity of sulfur and serious shuttling effect of intermediate polysulfides. Moreover, the areal capacity is usually restricted by the low areal sulfur loadings (1.0-3.0 mg cm-2). When the areal sulfur loading increases to a practically accepted level above 3.0-5.0 mg cm-2, the areal capacity and cycling life tend to become inferior. Herein, we report an effective polysulfide mediator composed of nitrogen-doped carbon nanotube (N-CNT) forest planted on cobalt nanoflowers (N-CNTs/Co-NFs). The abundant pores in N-CNTs/Co-NFs can allow a high sulfur content (78 wt %) and block the dissolution/diffusion of polysulfides via physical confinement, and the Co nanoparticles and nitrogen heteroatoms (4.3 at. %) can enhance the polysulfide retention via strong chemisorption capability. Moreover, the planted N-CNT forest on N-CNTs/Co-NFs can enable fast electron transfer and electrolyte penetration. Benefiting from the above merits, the sulfur-filled N-CNTs/Co-NFs (S/N-CNTs/Co-NFs) cathodes with high areal sulfur loadings exhibit low self-discharge rate, high areal capacity, and stable cycling performance.