Pseudohalide Anions to Suppress Oxidative Degradation for Efficient Formamidinium-Based Sn–Pb Halide Perovskite Solar Cells

Abstract

Although binary Sn-Pb perovskites possess optimal band gap approaching to the Shockley-Queisser limit efficiency, the enhancement on power conversion efficiency (PCE) of Sn-Pb perovskite solar cells (PSCs) is impeded by the detrimental oxidation of Sn²⁺. Herein, a novel and effective strategy is developed to introduce pseudohalide anion thiocyanate (SCN^-) with similar ionic radius to iodide to occupy the X-site of the perovskite lattice, thus restraining the rapid oxidation of Sn²⁺ to Sn⁴⁺. The incorporation of SCN^- into perovskite stabilizes the perovskite crystal structure thermodynamically and increases the adsorption-energy-barrier of oxygen molecules. The coordination between Sn²⁺ and SCN^- can reduce the defect density by healing the undercoordinated Sn²⁺ and suppressing the Sn and I vacancies. With the incorporation of SCN^-, the ion migration behavior and lattice strain associated with the defects are remarkably relaxed. The study on carrier dynamics based on steady-state and time-resolved photoluminescence suggests that the carrier lifetime and non-radiative recombination rate of SCN^- PSCs can be remarkably prolonged and depressed, respectively. As a result, FASn_0.5Pb_0.5I₃-based PSCs achieve a 14.5% increase in PCE, reaching 13.74% under AM 1.5G illumination. This strategy takes a noteworthy step toward high efficiency and high stability FA-based Sn-Pb PSCs.