In modern society, high-quality material development and a large stable supply are key to perform frontier research and development. However, there are negative issues to address to utilize high-quality resources with a large stable supply for research, such as economic accessibility, commercialization, and so on. One of the cutting-edge research fields, perovskite-related research, usually requires high-quality chemicals with outstanding purity (>99%). We developed an economically feasible PbI2 precursor with around 1/20 cost-down for perovskite/perovskite quantum dots through recrystallization and/or hydrothermal purification. Following the methodology, the quantum dots from both as-prepared and purified PbI2 demonstrated identical photophysical properties, with a photoluminescence quantum yield (PLQY) of 52.61% using the purified PbI2 vs. 45.83% PLQY using commercial PbI2. The role of hydrothermal energy was also checked against the problematic PbI2, and we checked whether the hydrothermal energy could contribute to the hindrance of undesired particle formation in the precursor solution, which enables them to form enlarged grain size from 179 ± 80 to 255 ± 130 nm for higher photoconversion efficiency of perovskite solar cells from 14.77 ± 1.82% to 15.18 ± 1.92%.

Current efforts to reduce the density of structural defects such as surface passivation, doping, and modified synthetic protocols have allowed us to grow high-quality perovskite nanocrystals (PNCs). However, the role of the purity of the precursors involved during the PNC synthesis to hinder the emergence of defects has not been widely explored. In this work, we analyzed the use of different crystallization processes of PbX2 (X = Cl– or I–) to purify the chemicals and produce highly luminescent and stable CsPbCl3–x Br x and CsPbI3 PNCs. The use of a hydrothermal (Hyd) process to improve the quality of the as-prepared PbCl2 provides blue-emitting PNCs with efficient ligand surface passivation, a maximum photoluminescence quantum yield (PLQY) of ∼ 88%, and improved photocatalytic activity to oxidize benzyl alcohol, yielding 40%. Then, the hot recrystallization of PbI2 prior to Hyd treatment led to the formation of red-emissive PNCs with a PLQY of up to 100%, long-term stability around 4 months under ambient air, and a relative humidity of 50–60%. Thus, CsPbI3 light-emitting diodes were fabricated to provide a maximum external quantum efficiency of up to 13.6%. We claim that the improvement of the PbX2 crystallinity offers a suitable stoichiometry in the PNC structure, reducing nonradiative carrier traps and so maximizing the radiative recombination dynamics. This contribution gives an insight into how the manipulation of the PbX2 precursor is a profitable and potential alternative to synthesize PNCs with improved photophysical features by making use of defect engineering.

All-inorganic lead-halide perovskite quantum dots (PQDs) (CsPbX3, where X is Cl, Br, or I) have been used successfully in optoelectronic applications, such as solar cells, light-emitting diodes, photocatalysts, and lasers. These PQDs work under electrochemical bias and/or illumination with charge separation/collection by interacting with the charge-transport medium. In this study, we discuss the spectroelectrochemical characteristics of PQDs to understand the oxidation and reduction processes that occur during photoinduced charge transport or charge injection under electrochemical conditions. We also found that the PQDs underwent irreversible transformation to the precursor state of plumbate complexes under electrochemical conditions. Furthermore, in situ spectroelectrochemical analysis demonstrated that hole-mediated electrochemical oxidation of PQDs resulted in their irreversible transformation. Finally, the results presented herein contribute to our understanding of the charge-transfer-mediated process in PQDs and enhance their application potential in optoelectronic devices.

Making high-quality raw materials is the key to open the versatile potential of next generation materials. All-inorganic CsPbX3 (X: Cl−, Br−, and/or I−) perovskite quantum dots (PQDs) have been applied in various optoelectronic devices, such as photocatalysis, hydrogen evolution, solar cells, and light-emitting diodes, due to their outstanding photophysical properties, such as high photoluminescence quantum yield (PLQY), absorption cross-section, efficient charge separation, and so on. Specifically, for further improvement of the PLQY of the PQDs, it is essential to diminish the non-radiative charge recombination processes. In this work, we approached two ways to control the non-radiative charge recombination processes through synthetic and post-synthetic processes. Firstly, we proposed how refinement of the conventional recrystallization process for PbI2 contributes to higher PLQY of the PQDs. Secondly, after halide exchange from CsPbI3 PQDs to CsPbBr3, through an in situ spectroelectrochemical setup, we monitored the positive correlation between bromide deposition of on the surface of the perovskite and photoluminescence improvement of the CsPbBr3 perovskite film through electrodeposition. These two strategies could provide a way to enhance the photophysical properties of the perovskites for application to various perovskite-based optoelectronic devices.

Organic-inorganic hybrid perovskites are widely utilized in solar driven chemistry such as photocatalysis, hydrogen evolution, and oxygen reduction. Hybrid perovskites contain various components with high polarity and/or charge values, which...