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, FASn0.5Pb0.5I3-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.
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