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 asselenized PdSe 2 is a promising material for optoelectronic application.
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.
While Li-S batteries are poised to be the next generation high-density energy storage devices, low sulfur utilization and slow rate performance have limited their practical applications. Here, we report the synthesis of monodispersed S8 nanoparticles (NPs) with different diameter and the nanosize dependent kinetic characteristics of the corresponding Li-S batteries. Most remarkably, 5 nm S NPs display the theoretical discharging/charging capacity of 1672 mAh g(-1) at 0.1 C rate and a discharge capacity of 1089 mAh g(-1) at 4 C.
Potassium has its unique advantages over lithium or sodium as a charge carrier in rechargeable batteries. However, progresses in K-ion battery (KIB) chemistry have so far been hindered by lacking suitable electrode materials to host the relatively large K ions compared to its Li and Na counterparts. Herein, molybdenum disulfide (MoS ) "roses" grown on reduced graphene oxide sheets (MoS @rGO) are synthesized via a two-step solvothermal route. The as-synthesized MoS @rGO composite, with expanded interlayer spacing of MoS , chemically bonded between MoS and rGO, and a unique nano-architecture, displays the one of the best electrochemical performances to date as an anode material for nonaqueous KIBs. More importantly, a combined K storage mechanism of intercalation and conversion reaction is also revealed. The findings presented indicate the enormous potential of layered metal dichalcogenides as advanced electrode materials for high-performance KIBs and also provide new insights and understanding of K storage mechanism.
A microscopic understanding of the growth mechanism of two-dimensional materials is of particular importance for controllable synthesis of functional nanostructures. Because of the lack of direct and insightful observations, how to control the orientation and the size of two-dimensional material grains is still under debate. Here we discern distinct formation stages for MoS2 flakes from the thermolysis of ammonium thiomolybdates using in situ transmission electron microscopy. In the initial stage (400 °C), vertically aligned MoS2 structures grow in a layer-by-layer mode. With the increasing temperature of up to 780 °C, the orientation of MoS2 structures becomes horizontal. When the growth temperature reaches 850 °C, the crystalline size of MoS2 increases by merging adjacent flakes. Our study shows direct observations of MoS2 growth as the temperature evolves, and sheds light on the controllable orientation and grain size of two-dimensional materials.
Solid electrolyte interphase (SEI) is an in situ formed thin coating on lithium ion battery (LIB) electrodes. The mechanical property of SEI largely defines the cycling performance and the safety of LIBs but has been rarely investigated. Here, we report quantitatively the Young's modulus of SEI films on MnO anodes. The inhomogeneity of SEI film in morphology, structure, and mechanical properties provides new insights to the evolution of SEI on electrodes. Furthermore, the quantitative methodology established in this study opens a new approach to direct investigation of SEI properties in various electrode materials systems.
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 assynthesized NiCoFe oxide catalysts indicates that Fe preferentially dopes into tetrahedral sites of the lattice, which induces high proportions of Ni 3+ and Co 2+ 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.
We report the synthesis of ultrafine S nanoparticles with diameter 10 ~ 20 nm via a membrane-assisted precipitation technique. The S nanoparticles were then coated with conducting poly (3,4-ethylenedioxythiophene) (PEDOT) to form S/PEDOT core/shell nanoparticles. The ultrasmall size of S nanoparticles facilitates the electrical conduction and improves sulfur utilization. The encapsulation of conducting PEDOT shell restricts the polysulfides diffusion, alleviates self-discharging and the shuttle effect, and thus enhances the cycling stability. The resulting S/PEDOT core/shell nanoparticles show initial discharge capacity of 1117 mAh g−1 and a stable capacity of 930 mAh g−1 after 50 cycles.
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