Chemical Synergic Stabilization of High Br‐Content Mixed‐Halide Wide‐Bandgap Perovskites for Durable Multi‐Terminal Tandem Solar Cells with Minimized Pb Leakage

Abstract

High Br‐content mixed‐halide perovskites with wide‐bandgap (WBG) of 1.6‐2.0 eV have showcased vast potential to be used in tandem solar cells. However, they often suffer from severe halide segregation, phase separation and ion migration issues, which would accelerate the decomposition of perovskites films, deteriorate the photovoltaic performance and even aggravate the lead leakage from damaged devices. Here, we report a novel chemical synergic interaction strategy to mitigate the abovementioned issues. A small amount of cationic β‐cyclodextrin, composed of multiple ammonium cations, chlorine ions and abundant hydroxyl functional groups, was introduced into WBG perovskites, which effectively stabilized the halide ions and homogenized the phase distribution, comprehensively passivated the defects,and efficiently immobilized the Pb2+ ions. Encouragingly, the cationic β‐cyclodextrin was universal and useful for different WBG perovskites, which favorably boosted the efficiencies by 10%‐36% and extended the device operational stability to 2680 h. The integrated four‐terminal or six‐terminal all‐perovskite tandem solar cells exhibited efficiencies up to 24.39% and 22.42%, respectively. We demonstrated the cationic β‐cyclodextrin‐assisted internal chemical encapsulation effectively prevented the Pb leakage from severely damaged devices with only 5.63 ppb Pb leaching out. The target tandem solar cells with cationic β‐cyclodextrin modification also realized a Pb sequestration efficiency of 93.4%.