Wei Lü

Abstract Palladium diselenide (PdSe 2 ), a thus far scarcely studied group‐10 transition metal dichalcogenide has exhibited promising potential in future optoelectronic and electronic devices due to unique structures and electrical properties. Here, the controllable synthesis of wafer‐scale and homogeneous 2D PdSe 2 film is reported by a simple selenization approach. By choosing different thickness of precursor Pd layer, 2D PdSe 2 with thickness of 1.2–20 nm can be readily synthesized. Interestingly, with the increase in thickness, obvious redshift in wavenumber is revealed by Raman spectroscopy. Moreover, in accordance with density functional theory (DFT) calculation, optical absorption and ultraviolet photoemission spectroscopy (UPS) analyses confirm that the PdSe 2 exhibits an evolution from a semiconductor (monolayer) to semimetal (bulk). Further combination of the PdSe 2 layer with Si leads to a highly sensitive, fast, and broadband photodetector with a high responsivity (300.2 mA W −1 ) and specific detectivity (≈10 13 Jones). By decorating the device with black phosphorus quantum dots, the device performance can be further optimized. These results suggest the as‐selenized PdSe 2 is a promising material for optoelectronic application.

A novel hierarchical nanotube array (NTA) with a massive layered top and discretely separated nanotubes in a core–shell structure, that is, nickel–cobalt metallic core and nickel–cobalt layered double hydroxide shell (NiCo@NiCo LDH), is grown on carbon fiber cloth (CFC) by template‐assisted electrodeposition for high‐performance supercapacitor application. The synthesized NiCo@NiCo LDH NTAs/CFC shows high capacitance of 2200 F g −1 at a current density of 5 A g −1 , while 98.8% of its initial capacitance is retained after 5000 cycles. When the current density is increased from 1 to 20 A g −1 , the capacitance loss is less than 20%, demonstrating excellent rate capability. A highly flexible all‐solid‐state battery‐type supercapacitor is successfully fabricated with NiCo LDH NTAs/CFC as the positive electrode and electrospun carbon fibers/CFC as the negative electrode, showing a maximum specific capacitance of 319 F g −1 , a high energy density of 100 W h kg −1 at 1.5 kW kg −1 , and good cycling stability (98.6% after 3000 cycles). These fascinating electrochemical properties are resulted from the novel structure of electrode materials and synergistic contributions from the two electrodes, showing great potential for energy storage applications.

Lithium sulfur batteries with high energy densities are promising next-generation energy storage systems. However, shuttling and sluggish conversion of polysulfides to solid lithium sulfides limit the full utilization of active materials. Physical/chemical confinement is useful for anchoring polysulfides, but not effective for utilizing the blocked intermediates. Here, we employ black phosphorus quantum dots as electrocatalysts to overcome these issues. Both the experimental and theoretical results reveal that black phosphorus quantum dots effectively adsorb and catalyze polysulfide conversion. The activity is attributed to the numerous catalytically active sites on the edges of the quantum dots. In the presence of a small amount of black phosphorus quantum dots, the porous carbon/sulfur cathodes exhibit rapid reaction kinetics and no shuttling of polysulfides, enabling a low capacity fading rate (0.027% per cycle over 1000 cycles) and high areal capacities. Our findings demonstrate application of a metal-free quantum dot catalyst for high energy rechargeable batteries.

A major challenge that prohibits the practical application of single/double-transition metal (3d-M) oxides as oxygen evolution reaction (OER) catalysts is the high overpotentials during the electrochemical process. Herein, our theoretical calculation shows that Fe will be more energetically favorable in the tetrahedral site than Ni and Co, which can further regulate their electronic structure of binary NiCo spinel oxides for optimal adsorption energies of OER intermediates and improved electronic conductivity and hence boost their OER performance. X-ray absorption spectroscopy study on the as-synthesized NiCoFe oxide catalysts indicates that Fe preferentially dopes into tetrahedral sites of the lattice, which induces high proportions of Ni3+ and Co2+ on the octahedral sites (the active sites in OER). Consequently, this material exhibits a significantly enhanced OER performance with an ultralow overpotential of 201 mV cm–2 at 10 mA cm–2 and a small Tafel slope of 39 mV dec–1, which are much superior to state-of-the-art Ni–Co based catalysts.