Methylammonium lead halide perovskites suffer from poor stability because of their high sensitivity to moisture. Inorganic material coatings of SiO2 are preferred for coupling with perovskites to improve their stability, whereas the conventional SiO2 formation method is unsuitable because it requires water. Here, a simple SiO2 generation method based on the high hydrolysis rate of tetramethyl orthosilicate in analytical-grade toluene was developed to avoid the addition of water and catalyst. As a result, SiO2-encapsulated CH3NH3PbBr3 quantum dots (MAPB-QDs/SiO2) were fabricated without decreasing the quantum yield. Photostability tests indicated that the MAPB-QDs/SiO2 samples were markedly more stable than the unencapsulated MAPB-QDs. The photoluminescence (PL) of the MAPB-QDs/SiO2 powders was maintained at 94.10% after 470 nm LED illumination for 7 h, which was much higher than the remnant PL (38.36%) of the pure MAPB-QD sample under a relative humidity of 60%. Similar test results were observed when the MAPB-QDs/SiO2 powders were incorporated into the poly(methyl methacrylate) films. The enhanced photostability is ascribed to the SiO2 barriers protecting the MAPB-QDs from degradation.
Under illumination of light-emitting diode (LED) or sunlight, the green color of all-inorganic CsPbBr perovskite nanocrystals (CPB-NCs) often quickly changes to yellow, followed by large photoluminescence (PL) loss. To figure out what is happening on CPB-NCs during the color change process, the morphology, structure, and PL evolutions are systematically investigated by varying the influence factors of illumination, moisture, oxygen, and temperature. We find that the yellow color is mainly originated from the large CPB crystals formed in the illumination process. With maximized isolation of oxygen for the sandwiched film or the uncovered film stored in nitrogen, the color change can be dramatically slowed down whether there is water vapor or not. Under dark condition, the PL emissions are not significantly influenced by the varied relative humidity (RH) levels and temperatures up to 60 °C. Under the precondition of oxygen or air, color change and PL loss become more obvious when increasing the illumination power or RH level, and the large-sized cubic CPB crystals are further evolved into the oval-shaped crystals. We confirm that oxygen is the crucial factor to drive the color change, which has the strong synergistic effect with the illumination and moisture for the degradation of the CPB film. Meanwhile, the surface decomposition and the increased charge trap states occurred in the formed large CPB crystals play important roles for the PL loss.
Traditional smart fluorescent materials, which have been attracting increasing interest for security protection, are usually visible under either ambient or UV light, making them adverse to the potential application of confidential information protection. Herein, we report an approach to realize confidential information protection and storage based on the conversion of lead-based metal-organic frameworks (MOFs) to luminescent perovskite nanocrystals (NCs). Owing to the invisible and controlled printable characteristics of lead-based MOFs, confidential information can be recorded and encrypted by MOF patterns, which cannot be read through common decryption methods. Through our conversion strategy, highly luminescent perovskite NCs can be formed quickly and simply by using a halide salt trigger that reacts with the MOF, thus promoting effective information decryption. Finally, through polar solvents impregnation and halide salt conversion, the luminescence of the perovskite NCs can be quenched and recovered, leading to reversible on/off switching of the luminescence signal for multiple information encryption and decryption processes.
We successfully prepared QDs incorporated into a silica/alumina monolith (QDs-SAM) by a simple sol-gel reaction of an Al-Si single precursor with CsPbBr QDs blended in toluene solution, without adding water and catalyst. The resultant transparent monolith exhibits high photoluminescence quantum yields (PLQY) up to 90 %, and good photostability under strong illumination of blue light for 300 h. We show that the preliminary ligand exchange of didodecyl dimethyl ammonium bromide (DDAB) was very important to protect CsPbBr QDs from surface damages during the sol-gel reaction, which not only allowed us to maintain the original optical properties of CsPbBr QDs but also prevented the aggregation of QDs and made the monolith transparent. The CsPbBr QDs-SAM in powder form was easily mixed into the resins and applied as color-converting layer with curing on blue light-emitting diodes (LED). The material showed a high luminous efficacy of 80 lm W and a narrow emission with a full width at half maximum (FWHM) of 25 nm.
Achieving good stability while maintaining excellent properties is one of the main challenges for enhancing the competitiveness of luminescent perovskite CsPbX 3 (X=Cl, Br, I) nanocrystals (NCs). Here, we propose a facile strategy to synthesize ceramic-like stable and highly luminescent CsPbBr 3 NCs by encapsulating them into silica derived from molecular sieve templates at high temperature (600-900 o C). The obtained CsPbBr 3 -SiO 2 powders not only show high photoluminescence quantum yield (~71%), but also show an exceptional stability comparable to the ceramic Sr 2 SiO 4 :Eu 2+ green phosphor. They can maintain 100% of their photoluminescence value under illumination on blue light-emitting diodes (LEDs) chips (20 mA, 2.7 V) for 1000 h, and can also survive in a harsh hydrochloric acid aqueous solution (1 M) for 50 days. We believe that the above robust stabilities will significantly enhance the potential of perovskite CsPbX 3 NCs to be practically applied in LEDs and backlight displays.
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