NiO Nanoparticle-Modified PTAA Hole Transport Layers for High-Efficiency and Stable Large-Area Perovskite Solar Cells

Abstract

The hole transport layer (HTL) plays a central role in governing charge extraction, efficiency, and long-term stability in perovskite solar cells (PSCs). Although poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) is widely used as an organic HTL, its limited hole mobility and thermal robustness restrict device durability and scalability. Here, we report a hybrid organic−inorganic HTL formed by incorporating NiO nanoparticles into PTAA to simultaneously improve charge transport and thermal stability. Comprehensive spectroscopic and electrical analyses reveal that NiO incorporation deepens the valence band position, enhances hole mobility, accelerates interfacial hole extraction, and suppresses carrier recombination in PTAA:NiO films. As a result, planar n−i−p PSCs employing PTAA:NiO (10 mg mL⁻¹) achieve a champion power conversion efficiency (PCE) of 20.76%, outperforming pristine PTAA-based devices (19.50%) while retaining 86.5% of their initial efficiency after 6000 h under ISOS-D-1 storage conditions. Importantly, NiO incorporation also improves module-level robustness by mitigating thermally induced interfacial degradation during high-temperature encapsulation. Scalable 10 × 10 cm² minimodules deliver a PCE of up to 14.18% and retain 85.1% of their initial performance after 5000 h. Furthermore, integrated minimodules successfully powered a standalone PM2.5 monitoring system under indoor illumination, highlighting the practical potential of hybrid-HTL PSCs for durable large-area photovoltaic and low-power Internet-of-Things applications.