Molecular Self-Assembly Regulated Dopant-Free Hole Transport Materials for Efficient and Stable n-i-p Perovskite Solar Cells and Scalable Modules

Angew Chem Int Ed Engl. 2022 Oct 17;61(42):e202210613. doi: 10.1002/anie.202210613. Epub 2022 Sep 20.

Abstract

Dopant-free organic hole transport materials (HTMs) remain highly desirable for stable and efficient n-i-p perovskite solar cells (pero-SCs) but rarely succeed. Here, we propose a molecular assembly strategy to overcome the limited optoelectronic properties of organic HTMs by precisely designing a linear organic small molecule BDT-DPA-F from the atomic to the molecular levels. BDT-DPA-F can assemble into a fibril network, showing an obviously improved hole mobility and decreased energy disorder. The resultant pero-SCs showed a promising efficiency of 23.12 % (certified 22.48 %), which is the highest certified value of pero-SCs with dopant-free HTMs, to date. These devices also showed a weak-dependence of efficiency on size, enabling a state-of-the-art efficiency of 22.50 % for 1-cm2 device and 20.17 % for 15.64-cm2 module. For the first time, the pero-SCs based on dopant-free HTMs realized ultralong stabilities with T80 lifetimes over 1200 h under operation or thermal aging at 85 °C.

Keywords: Dopant-Free Hole Transport Materials; Intermolecular Interactions; Operational and Thermal Stabilities; Perovskite Solar Cells; Self-Assembly.