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1.
J Am Chem Soc ; 144(12): 5552-5561, 2022 Mar 30.
Artigo em Inglês | MEDLINE | ID: mdl-35296136

RESUMO

Halide perovskites have the potential to disrupt the photovoltaics market based on their high performance and low cost. However, the decomposition of perovskites under moisture, oxygen, and light raises concerns about service lifetime, especially because degradation mechanisms and the corresponding rate laws that fit the observed data have thus far eluded researchers. Here, we report a water-accelerated photooxidation mechanism dominating the degradation kinetics of archetypal perovskite CH3NH3PbI3 in air under >1% relative humidity at 25 °C. From this mechanism, we develop a kinetic model that quantitatively predicts the degradation rate as a function of temperature, ambient O2 and H2O levels, and illumination. Because water is a possible product of dry photooxidation, these results highlight the need for encapsulation schemes that rigorously block oxygen ingress, as product water may accumulate beneath the encapsulant and initiate the more rapid water-accelerated photooxidative decomposition.

2.
Angew Chem Int Ed Engl ; 58(26): 8730-8735, 2019 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-31025792

RESUMO

Inorganic single crystals with anisotropic structures usually suffer from high brittleness and stiffness. Flexible polymers are used to replace inorganic crystals, but the hot-stretching-induced orientation process is tedious, and oriented molecular chains tend to revert to random coils during aging. To overcome these obstacles and using the similarities between sub-1 nm nanowires (NWs) and linear polymers, we successfully fabricated anisotropic, transparent, flexible, and stable (ATFS) NW films with great potential for optical applications through a wet-spinning method. The NW films show birefringence, and their birefractive index is higher than that of many polymers. They also showed polarized absorption of UV light and anisotropic scattering of visible light. The integrated films composed of NWs and quantum dots showed good fluorescence polarization. The tedious synthesis of quantum rods and fabrication of oriented polymer films can thus be avoided.

3.
Langmuir ; 35(6): 2146-2152, 2019 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-30616351

RESUMO

Color-changing materials have a variety of applications, ranging from smart windows to sensors. Here, we report deliquescent chromism of thin, color neutral films of nickel(II) iodide (NiI2) that are less than 10 µm thick. This behavior does not occur in the bulk material. Dark brown thin films of crystalline NiI2 turn clear when exposed to humidity and can be switched back to the dark state when mildly heated (>35 °C). This optical transition between dark and clear states of an NiI2 thin film is reversible with thermal cycling.

4.
ACS Appl Mater Interfaces ; 8(7): 4600-7, 2016 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-26771519

RESUMO

Surface oxidation of quantum dots (QDs) is one of the biggest challenges in quantum dot-sensitized solar cells (QDSCs), because it introduces surface states that enhance electron-hole recombination and degrade device performance. Protection of QDs from surface oxidation by passivating the surface with organic or inorganic layers can be one way to overcome this issue. In this study, solid-state QDSCs with a PbS QD absorber layer were prepared from thin mesoporous TiO2 layers by the successive ionic layer adsorption/reaction (SILAR) method. Spiro-OMeTAD was used as the organic p-type hole transporting material (HTM). The effects on the solar cell performance of passivating the surface of the PbS QDs with the tripeptide l-glutathione (GSH) were investigated. Current-voltage characteristics and external quantum efficiency measurements of the solar cell devices showed that GSH-treatment of the QD-sensitized TiO2 electrodes more than doubled the short circuit current and conversion efficiency. Impedance spectroscopy, intensity-modulated photovoltage and photocurrent spectroscopy analysis of the devices revealed that the enhancement in solar cell performance of the GSH-treated cells originates from improved charge injection from PbS QDs into the conduction band of TiO2. Time-resolved photoluminescence decay measurements show that passivation of the surface of QDs with GSH ligands increases the exciton lifetime in the QDs.

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