The role of chlorine in the formation process of "CH3NH3PbI3-xClx" perovskite
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AbstractCH3NH3PbI3-xClx is a commonly used chemical formula to represent the methylammonium lead halide perovskite fabricated from mixed chlorine- and iodine-containing salt precursors. Despite the rapid progress in improving its photovoltaic efficiency, fundamental questions remain regarding the atomic ratio of Cl in the perovskite as well as the reaction mechanism that leads to its formation and crystallization. In this work we investigated these questions through a combination of chemical, morphological, structural and thermal characterizations. The elemental analyses reveal unambiguously the negligible amount of Cl atoms in the CH3NH3PbI3-xClx perovskite. By studying the thermal characteristics of methylammonium halides as well as the annealing process in a polymer/perovskite/FTO glass structure, we show that the formation of the CH3NH3PbI3-xClx perovskite is likely driven by release of gaseous CH3NH3Cl (or other organic chlorides) through an intermediate organometal mixed halide phase. Furthermore, the comparative study on CH3NH3I/PbCl2 and CH3NH3I/PbI2 precursor combinations with different molar ratios suggest that the initial introduction of a CH3NH3+ rich environment is critical to slow down the perovskite formation process and thus improve the growth of the crystal domains during annealing; accordingly, the function of Cl- is to facilitate the release of excess CH3NH3+ at a relatively low annealing temperatures.
All Author(s) ListYu H., Wang F., Xie F., Li W., Chen J., Zhao N.
Journal nameAdvanced Functional Materials
Volume Number24
Issue Number45
PublisherJohn Wiley & Sons Ltd.
Place of PublicationUnited Kingdom
Pages7102 - 7108
LanguagesEnglish-United Kingdom
KeywordsAnnealing processes, Lead halide perovskite, Photovoltaics

Last updated on 2021-20-09 at 00:14