The efficiency and reproducibility of perovskite solar cells (PSCs) are significantly influenced by the purity of lead iodide (PbI2) in the raw materials used. Pb(OH)I has been identified as the primary impurity generated from PbI2in water-based synthesis. Consequently, a comprehensive investigation into the impact of Pb(OH)I impurities on film and device performance is essential. In this study, PbI2, with varying stoichiometries, was synthesized to examine the effects of different Pb(OH)I levels on perovskite device performance. The characterization results revealed that even trace amounts of Pb(OH)I impede the formation of precursor prenucleation clusters. These impurities also increase the energy barrier of the α-phase and facilitate the transition of the intermediate phase to the δ-phase. These effects result in poor perovskite film morphology and sub-optimal photovoltaic device performance. To address these issues, a cost-effective method for preparing high-stoichiometry PbI2was developed. The formation of Pb(OH)I was effectively inhibited through several strategies: adjusting solution pH and temperature, modifying material addition order, simplifying the precipitation–recrystallization process, and introducing H3PO2as an additive. These modifications enabled the one-step synthesis of high-purity PbI2. PSCs prepared using this newly synthesized high-stoichiometry PbI2demonstrated photovoltaic performance comparable to those fabricated with commercial PbI2(purity ≥ 99.999%). Our novel method offers a cost-effective alternative for synthesizing high-stoichiometry PbI2, thereby providing a viable option for the production of high-performance PSCs.
Jiaxu Yao,Liyan Yang,Feilong Cai,Yu Yan,Robert S. Gurney,Dan Liu,Tao Wang
We have fabricated planar heterojunction perovskite solar cells by one-step ultrasonic spray-coating of the perovskite precursor solution in air. Uniform perovskite films with high surface coverage can be prepared after optimization of the precursor solution and spray-coating parameters. We found that the purity of PbI2, although varying only from 98 to 99.9%, can significantly affect the crystallinity, grain size and boundaries of MAPbI3 films that were fabricated via one-step spray-coating, and ultimately determined the power conversion efficiency (PCE) of perovskite devices. PbI2 with a purity of 98% resulted in a low conversion of precursors to perovskites, whilst a high purity of 99.9% led to perovskites with a high crystallinity, large grain size and narrow grain boundaries. Our p–i–n type, planar heterojunction solar cell ITO/PEDOT:PSS/MAPbI3/PCBM/Ag made from MAI and 99.9% purity PbI2 achieved a maximum PCE of 12.6% without hysteresis, whereas the 98% purity PbI2-based device showed a low PCE of only 4.9% with the presence of hysteresis. However, the impacts of PbI2 purity on the device efficiency can be minimized by changing the deposition method from one-step spray-coating to a two-step spin casting approach.
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