Acidity Suppression of Hole Transport Layer via Solution Reaction of Neutral PEDOT:PSS for Stable Perovskite Photovoltaics

Poly(3,4-ethylenedioxythiophene): poly(4-styrenesulfonate) (PEDOT:PSS) is typically used for hole transport layers (HTLs), as it exhibits attractive mechanical, electrical properties, and easy processability. However, the intrinsically acidic property can degrade the crystallinity of perovskites, limiting the stability and efficiency of perovskite solar cells (PSCs). In this study, inverted CH₃NH₃PbI₃ photovoltaic cells were fabricated with acidity suppressed HTL. We adjusted PEDOT:PSS via a solution reaction of acidic and neutral PEDOT:PSS. And we compared the various pH-controlled HTLs for PSCs devices. The smoothness of the pH-controlled PEDOT:PSS layer was similar to that of acidic PEDOT:PSS-based devices. These layers induced favorable crystallinity of perovskite compared with acidic PEDOT:PSS layers. Furthermore, the enhanced stability of pH optimized PEDOT:PSS-based devices, including the prevention of degradation by a strong acid, allowed the device to retain its power conversion efficiency (PCE) value by maintaining 80% of PCE for approximately 150 h. As a result, the pH-controlled HTL layer fabricated through the solution reaction maintained the surface morphology of the perovskite layer and contributed to the stable operation of PSCs.