Controlling the growth of a SiO2 coating on hydrophobic CsPbBr3 nanocrystals towards aqueous transfer and high luminescence

Abstract

Silica coating can effectively solve the stability issue of lead halide perovskite nanomaterials. However, it is difficult to achieve aqueous SiO₂ coating on hydrophobic CsPbBr₃ nanocrystals (NCs). In this paper, the hydrolysis process of tetramethoxysilane was controlled to get a homogeneous SiO₂ coating or a NC/SiO₂ Janus structure. In step 1, the Cs₄PbBr₆ NCs were silanized using partially hydrolyzed tetramethoxysilane (PH-TMOS). During this process, the Si–OH groups which came from PH-TMOS were absorbed onto the surface of the Cs₄PbBr₆ NCs with the removal of hydrophobic oleic acid (OA) ligands. In step 2, phase transformation from Cs₄PbBr₆ to CsPbBr₃ occurred owing to the injection of water. Meanwhile, further hydrolysis of TMOS took place and generated cross-linked Si–O–Si. Because the silanization in step 1 created lots of growth sites, the condensation of SiO₂ was not limited to the interface between water and hexane. After growing for 12 h, the fully covered CsPbBr₃@SiO₂ capsules were prepared. The anion exchange reactions of the CsPbBr₃@SiO₂ capsules were studied. Only one even and symmetric PL peak was apparent during the anion exchange process, which was different from the bare CsPbBr₃ NCs. This result demonstrated that the SiO₂ shell can act as a buffer layer to block the direct contact of CsPbBr₃ with the excess PbBr₂ precursor in solution. Compared with the CsPbBr₃ NCs, CsPbBr₃@SiO₂ showed better stability in polar solvent and air. A bright green emission was also observed under UV light after 90 days. The successful preparation of CsPbBr₃@SiO₂ capsules with enhanced stability paves the way for the further development of lead halide perovskite nanomaterials.