Amorphous Modulation of Atomic Nb-O/N Clusters with Asymmetric Coordination in Carbon Shells for Advanced Sodium-Ion Hybrid Capacitors.

Anode materials with excellent properties have become the key to develop sodium-ion hybrid capacitors (SIHCs) that combine the advantages of both batteries and capacitors. Amorphous modulation is an effective strategy to realize high energy/power density in SIHCs. Herein, atomically amorphous Nb-O/N clusters with asymmetric coordination are in situ created in N-doped hollow carbon shells (Nb-O/N@C). The amorphous clusters with asymmetric Nb-O3/N1 configurations have abundant charge density and low diffusion energy barriers, which effectively modulate the charge transport paths and improve the reaction kinetics. The clusters are also enriched with unsaturated vacancy defects and isotropic ion-transport channels, and their atomic disordering exhibits high structural stress buffering, which are strong impetuses for realizing bulk-phase-indifferent ion storage and enhancing the storage properties of the composite. Based on these features, Nb-O/N@C achieves notably improved sodium-ion storage properties (reversible capacity of 240.1 mAh g-1 at 10.0 A g-1 after 8000 cycles), and has great potential for SIHCs (230 Wh Kg-1 at 4001.5 W Kg-1). This study sheds new light on developing high-performance electrodes for sodium-ion batteries and SIHCs by designing amorphous clusters and asymmetric coordination.

Phase-Selective Synthesis of Cobalt Sulfide Heterostructure Catalysts as Efficient Counter Electrodes in Dye-Sensitized Solar Cells.

Developing a cost-saving, high-efficiency, and simple synthesis of counter electrode (CE) material to replace pricy Pt for dye-sensitized solar cells (DSSCs) has become a research hotspot. Owing to the electronic coupling effects between various components, semiconductor heterostructures can significantly enhance the catalytic performance and endurance of counter electrodes. However, the strategy to controllably synthesize the same element in several phase heterostructures used as the CE in DSSCs is still absent. Here, we fabricate well-defined CoS2 /CoS heterostructures and use them as CE catalysts in DSSCs. The as-designed CoS2 /CoS heterostructures display high catalytic performance and endurance for the triiodide reduction in DSSCs thanks to the combined and synergistic effects. As a result, a DSSC with CoS2 /CoS achieves a high energy conversion with an efficiency of 9.47 % under standard simulated solar radiation, surpassing that of pristine Pt-based CE (9.20 %). Besides, the CoS2 /CoS heterostructures possess a quick activity initiation process and extended stability, broadening their potential applications in various areas. Therefore, our proposed synthetic approach could offer new insights for synthesizing functional heterostructure materials with improved catalytic activities in DSSCs.

Photovoltaic Counter Electrodes: An Alternative Approach to Extend Light Absorption Spectra and Enhance Performance of Dye-Sensitized Solar Cells.

If counter electrodes (CEs) could also contribute to light harvesting in dye-sensitized solar cells (DSSCs), then the power conversion efficiency (PCE) of DSSCs would be further boosted without changing the device structure. Nearly monodispersed Ag2 Se nanocrystals with a bandgap of 1.62 eV (∼765 nm) were synthesized via a one-pot process, and Ag2 Se CEs were fabricated by using a spin-coating and annealing process. Incident photon-to-current conversion efficiency and photocurrent spectra indicated that Ag2 Se CEs can generate the electricity by harvesting more visible light, which could not be absorbed by dye-sensitized photoanodes. Thus, compared to Pt CE (7.57 %), the DSSC based on Ag2 Se CE exerted a higher PCE of 8.06 %. The development of photovoltaic CEs may offer an alternative way to promote the performance and competitiveness of DSSCs.

Highly active nanostructured CoS2/CoS heterojunction electrocatalysts for aqueous polysulfide/iodide redox flow batteries.

Aqueous polysulfide/iodide redox flow batteries are attractive for scalable energy storage due to their high energy density and low cost. However, their energy efficiency and power density are usually limited by poor electrochemical kinetics of the redox reactions of polysulfide/iodide ions on graphite electrodes, which has become the main obstacle for their practical applications. Here, CoS2/CoS heterojunction nanoparticles with uneven charge distribution, which are synthesized in situ on graphite felt by a one-step solvothermal process, can significantly boost electrocatalytic activities of I-/I3- and S2-/Sx2- redox reactions by improving absorptivity of charged ions and promoting charge transfer. The polysulfide/iodide flow battery with the graphene felt-CoS2/CoS heterojunction can deliver a high energy efficiency of 84.5% at a current density of 10 mA cm-2, a power density of 86.2 mW cm-2 and a stable energy efficiency retention of 96% after approximately 1000 h of continuous operation.

Synergistically Enhanced Electrochemical Performance of Ni3S4-PtX (X = Fe, Ni) Heteronanorods as Heterogeneous Catalysts in Dye-Sensitized Solar Cells.

Platinum (Pt)-based alloys are considerably promising electrocatalysts for the reduction of I-/I3- and Co2+/Co3+ redox couples in dye-sensitized solar cells (DSSCs). However, it is still challenging to minimize the dosage of Pt to achieve comparable or even higher catalytic efficiency. Here, by taking full advantages of the Mott-Schottky (M-S) effect at the metal-semiconductor interface, we successfully strategize a low-Pt-based M-S catalyst with enhanced electrocatalytic performance and stability for the large-scale application of DSSCs. The optimized M-S electrocatalyst of Ni3S4-Pt2X1 (X = Fe, Ni) heteronanorods is constructed by rationally controlling the ratio of Pt to transition metal in the hybrids. It was found that the electrons transferred from Ni3S4 to Pt2X1 at their interface under the Mott-Schottky effect result in the concentration of electrons onto Pt2X1 domains, which subsequently accelerates the regeneration of both I-/I3- and Co2+/Co3+ redox shuttles in DSSCs. As a result, the DSSC with Ni3S4-Pt2Fe1 manifests an impressive power conversion efficiency (PCE) of 8.79% and 5.56% for iodine and cobalt-based electrolyte under AM1.5G illumination, respectively. These PCEs are obviously superior over those with Ni3S4-Pt, PtFe, Ni3S4, and pristine Pt electrodes. The strategy reported here is able to be further expanded to fabricate other low-Pt-alloyed M-S catalysts for wider applications in the fields of photocatalysis, water splitting, and heterojunction solar cells.

Colloidal synthesis of wurtz-stannite Cu2CdGeS4 nanocrystals with high catalytic activity toward iodine redox couples in dye-sensitized solar cells.

Wurtz-stannite Cu2CdGeS4 nanocrystals were synthesized via a facile hot-injection method at a low temperature. They exhibited low charge transfer resistance at the electrolyte-electrode interface and high electrocatalytic activity for the reduction of I3(-) in dye-sensitized solar cells (DSSCs). Moreover, this DSSC showed a power conversion efficiency of 7.67%, comparable to the Pt-based device (7.54%).

0D to 1D Switching of Hybrid Polyoxometalate Assemblies at the Nanoscale by Using Molecular Control.

Watered down: Polyoxometalate (POM) hybrids based on [C16 H36 N]4 [SiW11 O40 (SiCH2 CH2 CH2 NH2 ⋅HCl)2 ] covalently functionalized with different lengths of alkyl chains (n=0, 5, or 10) terminated with azobenzene moieties have been successfully prepared. The assembly behavior of these POMs can be affected by hydrophobic and π-π interactions by finely tuning the lengths of the alkyl chains in different ratios of CH3 CN/H2 O.