Highly Efficient and Stable Roll‐to‐Roll Coated Perovskite Solar Cells Enabled by Antisolvent Vapor‐Assisted Crystallization

ABSTRACT

A key challenge in roll‐to‐roll (R2R) perovskite solar cell (PSC) manufacturing is translating crystallization‐control methods developed for laboratory‐scale spin coating to scalable processes. Liquid antisolvent baths suffer from process drift due to contamination and generate substantial solvent waste, while gas‐assisted quenching induces rapid nucleation with limited control over grain growth. Here, antisolvent vapor‐assisted crystallization (AVAC) is demonstrated as a scalable strategy for controlling perovskite crystallization during R2R slot‐die coating under ambient conditions. By regulating antisolvent vapor partial pressure within the coating zone, AVAC controls host‐solvent extraction, limits moisture exposure, and promotes grain growth. One‐step R2R coating of Cs ₀ . ₁₂ FA ₀ . ₈₈ PbI ₃ films using AVAC produces pinhole‐free, α‐phase films with grain sizes exceeding 500 nm. Corresponding PSCs with evaporated gold electrodes achieve champion power conversion efficiencies (PCEs) of 18.3%, and 15.2% for fully R2R‐processed PSCs with a carbon electrode. The latter retain 97% of their initial PCE after more than 550 h of maximum power point tracking under 1000 W m ^{− 2} illumination in an inert atmosphere at 38°C ± 2°C and < 1% relative humidity. This performance ranks among the highest reported for R2R‐processed PSCs. Technical challenges associated with antisolvent properties for AVAC are discussed and suitable candidates for R2R manufacturing are identified.