• Energy Research

AbstractTin halide perovskites attract incremental attention to deliver lead‐free perovskite solar cells. Nevertheless, disordered crystal growth and low defect formation energy, related to Sn(II) oxidation to Sn(IV), limit the efficiency and stability of solar cells. Engineering the processing from perovskite precursor solution preparation to film crystallization is crucial to tackle these issues and enable the full photovoltaic potential of tin halide perovskites. Herein, the ionic liquid n‐butylammonium acetate (BAAc) is used to tune the tin coordination with specific O…Sn chelating bonds and NH…X hydrogen bonds. The coordination between BAAc and tin enables modulation of the crystallization of the perovskite in a thin film. The resulting BAAc‐containing perovskite films are more compact and have a preferential crystal orientation. Moreover, a lower amount of Sn(IV) and related chemical defects are found for the BAAc‐containing perovskites. Tin halide perovskite solar cells processed with BAAc show a power conversion efficiency of over 10%. This value is retained after storing the devices for over 1000 h in nitrogen. This work paves the way toward a more controlled tin‐based perovskite crystallization for stable and efficient lead‐free perovskite photovoltaics.

AbstractThe long‐term stability issue of halide perovskite solar cells hinders their commercialization. The residual stress–strain affects device stability, which is derived from the mismatched thermophysical and mechanical properties between adjacent layers. In this work, we introduced the Rb2CO3 layer at the interface of SnO2/perovskite with the hierarchy morphology of snowflake‐like microislands and dendritic nanostructures. With a suitable thermal expansion coefficient, the Rb2CO3 layer benefits the interfacial stress relaxation and results in a compressive stress–strain in the perovskite layer. Moreover, reduced nonradiative recombination losses and optimized band alignment were achieved. An enhancement of open‐circuit voltage from 1.087 to 1.153 V in the resultant device was witnessed, which led to power conversion efficiency (PCE) of 22.7% (active area of 0.08313 cm2) and 20.6% (1 cm2). Moreover, these devices retained 95% of its initial PCE under the maximum power point tracking (MPPT) after 2700 h. It suggests inorganic materials with high thermal expansion coefficients and specific nanostructures are promising candidates to optimize interfacial mechanics, which improves the operational stability of perovskite cells.

Daily temperature variations induce phase transitions and lattice strains in halide perovskites, challenging their stability in solar cells. We stabilized the perovskite black phase and improved solar cell performance using the ordered dipolar structure of β-poly(1,1-difluoroethylene) to control perovskite film crystallization and energy alignment. We demonstrated p-i-n perovskite solar cells with a record power conversion efficiency of 24.6% over 18 square millimeters and 23.1% over 1 square centimeter, which retained 96 and 88% of the efficiency after 1000 hours of 1-sun maximum power point tracking at 25° and 75°C, respectively. Devices under rapid thermal cycling between −60° and +80°C showed no sign of fatigue, demonstrating the impact of the ordered dipolar structure on the operational stability of perovskite solar cells.