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Enhancing Supersaturation Processes in the Fabrication of Perovskite Solar Cells Using Ionic Liquids

Rajabzadeh, Saeed | 2025

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  1. Type of Document: Ph.D. Dissertation
  2. Language: Farsi
  3. Document No: 58730 (48)
  4. University: Sharif University of Technology
  5. Department: Institute for Nanoscience and Nanotechnology
  6. Advisor(s): Taghavinia, Nima; Tajabadi, Fariba
  7. Abstract:
  8. Perovskite solar cells (PSCs) have emerged as a promising photovoltaic technology due to their high power conversion efficiency, ease of fabrication, relatively low production cost, and compatibility with various scalable deposition techniques. Nevertheless, several critical challenges including sensitivity to moisture and ambient oxygen, long-term instability, and the widespread use of toxic anti-solvents during film fabrication still hinder the large-scale commercialization of PSCs. Achieving perovskite layers with high crystalline quality, uniform and stable morphology under ambient conditions, and without employing harmful chemicals is a key bottleneck for industrial development. The main objective of this thesis is to develop an optimized and innovative strategy for controlling supersaturation and fabricating high-quality perovskite layers using green, non-toxic ionic-liquid-based solvents. To this end, dodecyl pyridinium chloride (DPCl) was introduced, for the first time, as an additive into an ionic-liquid-based MAPbI₃ perovskite ink containing methylammonium acetate (MAAc), enabling anti-solvent-free processing. The incorporation of DPCl led to a substantial improvement in film morphology and crystalline structure, increasing the grain size to above 1 μm and significantly suppressing structural defects. Electrochemical impedance spectroscopy further revealed a ~38% enhancement in charge recombination resistance. Two deposition techniques, spin coating and blade coating, were investigated, with a particular emphasis on blade coating because of its higher potential for scalable and industrial manufacturing. Blade-coating conditions for ionic-liquid-containing perovskite inks were systematically optimized under controlled ambient conditions (relative humidity > 40% and room temperature) using green solvents. Under these optimized conditions, DPCl-modified MAPbI₃ layers resulted in improved film quality and device performance, achieving a power conversion efficiency of about 16% under realistic ambient conditions. A short-circuit current density (Jsc) of up to 21.6 mA/cm², an open-circuit voltage (Voc) of ~1.08 V, and a fill factor (FF) of 68% were obtained. Stability tests carried out in ambient air confirmed stable device operation for more than 300 hours with no significant degradation. Moreover, eliminating the hole transport layer and replacing expensive metal electrodes such as gold with carbon electrodes substantially reduced fabrication costs and enhanced the commercial viability of the technology. Overall, this thesis proposes a green, cost-effective, and industrially scalable route to perovskite film fabrication, representing a meaningful step toward the commercialization and broader industrial adoption of perovskite solar cells
  9. Keywords:
  10. Perovskite-Based Solar Cell ; Scalability ; Supersaturation ; Ionic Liquids ; Scalable Deposition ; Chloride Additives ; Methylammonium Acetate

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