Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.276
Publication date: 18th December 2023
Metallic lead is easily formed in films due to decomposition of residual PbI2 in excess lead iodide-incorporated perovskites under light or X-ray irradiation. Pb0 is a typical intrinsic defect which limits mainly the stability of this type of solar cell [1]. A common strategy to heal the defective perovskite is passivation with thiol (-SH) containing ligands which can bind strongly to Pb0 or Pb2+ [2], and reduce directly -or indirectly- Pb0 impurities. Even though a large number of multifunctional compounds, bearing thiol groups, has been tested successfully, there is a lack of consensus on the origins of Pb0 elimination through this approach [3,4].
In this work, we used a model compound, 2-diethylaminoethanethiol (DEAET) in a very low concentration, as a top surface passivator of 10% PbI2 excessive-FAPbI3 and confirmed the enhanced radiative recombination through photoluminescence spectroscopy. XPS analysis has shown a total elimination of Pb0. When depositing DEAT ontop of PbI2 as a reference experiment, XPS revealed a simultaneous down shift for both Pb and I peaks, pointing to a clear chemical interaction of DEAT with PbI2; this interaction causes the disappearance of metallic lead from FAPI films. On the other hand, liquid 1H and 13C NMR, upon titration of DEAT with PbI2, has shown that the starting thiol disappears over time and a disulfide (oxidized form of the thiol) appears; finally, only the complex of PbI2 with the disulfide exists. The findings of this study point to the necessity of understanding the redox chemistry of thiol-based salts that dictates the passivation of PbI2-excessive FAPI perovskite.
We acknowledge the financial support from the Hellenic Foundation for Research and Innovation (HFRI) under the “First Call for H.F.R.I. Research Projects to support Faculty members and Researchers and the procurement of high-cost research equipment grant” (Project Number: 1027). We also thank the European Research Council (ERC) through Consolidator Grant (818615-MIX2FIX).
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