Publication date: 11th March 2026
Perovskite solar cells (PSCs) have nowadays demonstrated remarkable power conversion efficiency (PCE), exceeding 27% in lab scale. However, their scalable manufacturing under ambient conditions remains a significant challenge, with anti-solvent quenching of perovskite precursor wet film to be considered an integral manufacturing step for attaining high-quality perovskite active layers. In parallel, the conventional noble-metal hole-transport-layer-based (HTL-based) architectures of perovskite photovoltaics are the main designs to enable the record efficiencies, but yet incompatible with large-scale manufacturing. As an alternative, the carbon-based HTL-free design is considered the frontrunner to the photovoltaics market, providing lower performance but significantly higher stability, cost-effectiveness and full compatibility with printing processing on an industrial level. The present work deals with the development of single-crystal-derived perovskite precursor inks and their solution chemistry optimization to attain high performance in n-i-p carbon-based HTL-free solar cells without an anti-solvent processing step. More specifically, methylamine (CH3NH2)-diffusion route is employed to engineer the perovskite precursor solution to control phase transformation of the 3D black single-crystal perovskite into a clear, yellow, viscous liquid intermediate, preserving structural coordination, avoiding full decomposition into a random ionic solution. By optimizing this intermediate-phase through systematic tuning of the CH3NH2:CH3NH3PbI3 molar ratio, the intermediate-phase chemistry, nucleation and crystallization kinetics are controlled, leading to uniform, pinhole-free perovskite films, with μm-sized grains under ambient air. To this end, ambient-air processed C-based HTL-free PSCs with PCEs up to 16% and with enhanced stability are fabricated. Notably, the unencapsulated devices show a remarkable stability under dark storage aging (ISOS-D-1 protocol conditions), surpassing the limit of 1000 h of aging without detecting any degradation in their light-to-electricity conversion efficiency. This work elucidates the fundamental role of intermediate-phase chemistry in perovskite precursor inks and establishes a robust, antisolvent-free pathway toward highly efficient and stable PSCs manufacturing under ambient conditions.
The work is supported by the action: "Promotion of quality, innovation and extroversion in universities (ID 16289)", "SUB1.1 Clusters of Research Excellence - CREs" and funded by the Special Account of the Ministry of Education, Religious Affairs and Sports within the framework of the National Recovery and Resilience Plan “Greece 2.0”, with funding from the European Union – NextGenerationEU and co-financing from national resources (National Public Investments Program – VAT contribution).
Funding: This research was funded by the European Union – NextGenerationEU through the Greece 2.0 National Recovery and Resilience Plan, under the program “SUB 1.1 – Clusters of Research Excellence (CREs)”
[Project: Bifacial Photovoltaic modules made of perovskite materials with variable transparency for greenhouse applications (BiPSC4Agri), Grant No. ΥΠ3ΤΑ-0559425].
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