Three types of next generation batteries are currently being envisaged among the international community: metal-air batteries, multivalent cation batteries and all-solid-state batteries. These battery designs require high-performance, safe and cost effective electrolytes that are compatible with optimized electrode materials. Solid electrolytes have not yet been extensively employed in commercial batteries as they suffer from poor ionic conduction at acceptable temperatures and insufficient stability with respect to lithium-metal. Here we show a novel type of glasses, which evolve from an antiperovskite structure and that show the highest ionic conductivity ever reported for the Li-ion (25 mS cm À1 at 25 C). These glassy electrolytes for lithium batteries are inexpensive, light, recyclable, non-flammable and non-toxic.Moreover, they present a wide electrochemical window (higher than 8 V) and thermal stability within the application range of temperatures.
Herein, we report the variation of localized surface plasmon resonance (LSPR) of gold nanoparticle (NP) arrays covered by poly(3,4-ethylenedioxythiophene) (PEDOT) as a function of the electronic state of the polymer. Giant shifts and fine-tuning of the LSPR of gold NPs surrounded by PEDOT/sodium docecyl sulfate have been achieved. The color variations of plasmonic/conducting polymer (CP) devices are given not only by changes of the optical properties of the CP upon doping but also by a close synergy of the optical properties of CP and NP. Such systems can considerably extend the field of CP-based electrochromic devices.
The functionalization of electrode materials through diazonium electroreduction using a heteroaromatic compound, without phenyl groups, has been investigated for the first time. The electrochemical reduction of 2-aminoterthiophenyldiazonium cation, generated in situ, coats the electrode (glassy carbon (GC), gold or platinum) with an ultrathin organic layer, shown by X-ray photoelectron spectroscopy (XPS) of that deposited on gold to consist of terthiophene or oligothiophene. The coating is electroactive at potential close to that of terthiophene in solution. The electrochemical response of the modified GC electrode in the presence of various reversible redox couples shows that the attached layer acts as a conductive switch. It behaves as a barrier to electron transfer when the standard redox potential is below 0.5 V/SCE; in this case diode-like behavior is observed. However, for more oxidizing redox probes the layer can be considered as transparent and no barrier effect is observed. The layer deposited on a platinum ultramicroelectrode (UME) behaves similarly to that obtained on the large GC electrode. Scanning electrochemical microscopy (SECM) can be performed using this electroswitchable modified platinum UME which can act as a filter toward competitive redox exchange pathways.
Control of the optical properties of metallic nanoparticles (NP) is realized using an electrochemical switch consisting of a thin layer of conducting polymer (CP). It is shown that the quenching of localized surface plasmon (LSP) sustained by oblate particles depends of the frequency of the LSP resonance. This effect is attributed to the variation of the CP dielectric function with wavelength. As a consequence, prolate arrays show total quenching of the LSP resonance along the major axis of the particles whereas modulation and moderate damping are observed along the minor axis. Combining electroactive conducting polymer and prolate NP makes it possible to design active plasmonic devices with anisotropic optical response upon CP switching. In the present case, such devices can be used as active filters or polarizers.
The electrochemical reduction of diazonium salts, generated in situ, from 2-(4-aminophenyl)-3,4-ethylenedioxythiophene and two new amino functionalized π-conjugated oligomers incorporating 3,4-ethylenedioxythiophene (EDOT) and thiophene units, has been investigated. It coats the electrodes (glassy carbon (GC), gold or ITO) with an ultrathin organic layer (less than 10 nm thickness). The X-ray photoelectron spectroscopy (XPS) investigations confirm the presence of the starting oligomers deposited on the surface. As an important result, EDOT-based oligomer grafting was achieved on those surfaces which may be of general use as adhesion primer layers in all devices using PEDOT type materials. Furthermore, the coating is electroactive and the electrochemical investigations exhibit redox signal at potentials close to that obtained for short oligoEDOT in solution. The electrochemical responses of the modified GC electrodes were further studied in the presence of various reversible redox probes, showing that the attached layer acts as a conductive switch. The switching potential of the generated layer depends on the configuration of the starting oligomers and more precisely on the relative location of the EDOT unit. Such layer behave as a barrier to electron transfer when the standard redox potential of the redox probe is below the layer switching potential; in this case, a positive potential shift of the probe oxidation peak and a diode-like behavior are observed. However, for redox probes with redox potentials above the switching potential of the grafted film, the layer is transparent toward electron transfer, and no barrier effect is observed.
We have analyzed the hopping movement of a new ionic solid electrolyte by calculating defect formation energies and activation barriers. The role of the lattice during diffusion was established. Thermodynamic properties were determined by means of first principles and phonon calculations at working temperatures. The new solid electrolyte, an antiperovskite, Li3-2xMxAO (in which M is a higher valent cation like Ca2+ or Mg2+ and A is a halide like Cl- or Br- or a mixture of halides), was studied either pure or doped. Moreover, we present experimental ionic conductivity data for these novel solid state ionic conductors for the doped and the pure solid electrolyte from room temperature and up to ∼253 °C. In this paper, we compare the ionic conductivity of the latter solid electrolyte with other fast ionic conductors.
A bottom-up electrochemical process for fabricating conjugated ultrathin layers with tailored switchable properties is developed. Ultrathin layers of covalently grafted oligo(bisthienylbenzene) (oligo(BTB)) are used as switchable organic electrodes, and 3,4-ethylenedioxythiophene (EDOT) is oxidized on this layer. Adding only a few (less than 3) nanometers of EDOT moieties (5 to 6 units ) completely changes the switching properties of the layer without changing the surface concentration of the electroactive species. A range of new materials with tunable interfacial properties is created. They consist of oligo(BTB)-oligo(EDOT) diblock oligomers of various relative lengths covalently grafted onto the underlying electrode. These films retain reversible redox on/off switching and their switching potential can be finely tuned between +0.6 and -0.3 V/SCE while the overall thickness remains below 11 nm.
To make the concept of building-integrated solar cells viable, the latter should possess an increased tolerance towards light incident angle and intensity that naturally change along the day, among other required properties. In this work, three solar cell technologies as candidates for building-integrated applications are compared regarding their normalized average efficiency as a function of light intensity and incident angle. The mechanisms that lead to higher efficiency independence are evidenced by comparing several cell designs for dye-sensitized solar cells (DSC) and perovskite solar cells (PSC). By doing so, it was found that superior efficiency independence towards tilted light is obtained for PSC with more transparent active layers due to optical path lengthening (OPL), while DSC were found to exhibit OPL in standard configuration. All cells show a fairly stable efficiency evolution when light intensity was reduced, while at lower light intensity PSC slightly outperform DSC. The almost constant relative efficiency evolution of silicon heterojunction (SHJ) solar cells is a very interesting outcome of this work and so far, efficiency evolution of such SHJ under low light intensity have not been reported in the literature to the best of our knowledge.
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