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CsPbI 2Br薄膜在大气环境下制备存在覆盖率低、结晶质量差和结构稳定性差等问题. 本文提出了一种动态热风辅助再结晶策略(dynamic hot-air assisted recrystallization, DHR), 在相对湿度大于60% (>60% RH)的大气环境下, 制备出高覆盖率、(100)择优取向、大尺寸晶粒、结构稳定、光电性能好的CsPbI 2Br薄膜. 这是由于动态热风过程能够有效提高薄膜的覆盖率和获得(100)择优取向的结晶, 但晶粒尺寸会显著减小( R ave= 0.32 μm)并伴随着大量的晶界形成, 从而加剧载流子的非辐射复合( τ ave= 99 ns); 而通过再结晶过程, 可进一步提高(100)择优取向的结晶和显著增大晶粒尺寸( R ave= 2.63 μm), 从而提高薄膜的光致发光强度和荧光寿命( τ ave= 118 ns). 由DHR策略制备的未封装CsPbI 2Br太阳能电池具备高光电转换效率(power conversion efficiency, PCE = 17.55%)、低迟滞因子(hysteresis index, HI = 2.34%)和长期的储存稳定性(air, >60% RH, 40天, 初始PCE的96%)等特性.CsPbI 2Br thin films prepared in ambient air are susceptible to humidity, resulting in low coverage, poor crystallization quality, numerous pinholes, and easy transformation into non perovskite phases. To overcome the troubles of pervoksite fabrication in ambient air, a feasible way is to reduce the moisture around the films as much as possible according to dynamic hot-air assisted strategy. However, the hot air accelerates the evaporation rate of solvent, resulting in the decrease of grain size. In order to improve the crystal growth and long-term stability in dynamic hot-air assisted strategy, in this work, we present a dynamic hot-air assisted recrystallization (DHR) strategy to prepare high-quality CsPbI 2Br thin films in ambient air (i.e. the CsPbI 2Br thin films prepared via dynamic hot-air strategy are recrystallized by using a green solvent (methylamine acetate) with high viscosity coefficient). Under ambient air with high humidity (RH>60%), the CsPbI 2Br thin film with high coverage, (100) preferred orientation, large average grain size, and stable structure is prepared via DHR strategy. The dynamic hot-air process can effectively reduce the moisture around the film and increase the nucleation sites in the precursor solution, thereby improving the coverage of the film. However, this process inevitably results in the significant decrease of grain size ( R ave= 0.32 μm) (i.e. more grain boundaries), exacerbating non-radiative recombination of carriers associated with trap states at these boundaries. The high coverage increases the grain-to-grain contact area, facilitating complete recrystallization. Thus, the recrystallization process can significantly increase the grain size ( R ave= 2.63 μm) and obtain a (100) preferred orientation ( I (110)/ I (200)= 0.006), resulting in high photoluminescence intensity and long fluorescence lifetime (118 ns). The unencapsulated CsPbI 2Br perovskite solar cell (PSC) optimized via DHR strategy with low hysterescence factor (2.34%) and high repeatability exhibits a high power conversion efficiency (PCE = 17.55%), which is higher than those of most CsPbI 2Br PSCs prepared in ambient air and gloveboxes previously reported. Moreover, the unencapsulated CsPbI 2Br PSC possesses an excellent storage stability under ambient air with high humidity (RH > 60%), remaining 96% of the original PCE after aging 40 days. This provides a promising approach for achieving high-performance and long-term stable CsPbI 2Br films under ambient air with high humidity, which is expected to promote the commercialization process of perovskite/silicon tandem cells and semi-transparent devices.
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Keywords:
- CsPbI2Br/
- dynamic hot-air assisted recrystallization/
- ambient air/
- photoelectric performance
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Sample A1 τ1/ns A2 τ2/ns τave/ns Control 0.92 6.45 0.08 118 75 REC 0.91 7.35 0.09 160 112 DHA 0.71 2.77 0.29 105 99 DHR 0.69 9.36 0.31 135 118 年份 制备环境 策略 效率/% 稳定性 文献 2022 N2 Doping 16.20 88.6%, 42 d (air, 30% RH) [35] 2023 N2 Interface engineering 17.33 88.7%, 42 d (air, 10% RH) [36] 2023 N2 Doping 17.70 97%, 42 d (air, 10% RH) [37] 2019 Air, 25%—35% RH DHA 14.85 90%, 17 d (air, 85 ℃) [18] 2020 Air, 30% RH Precursor engineering 16.14 93%, 35 d (air, 30% RH) [17] 2021 Air, 35% RH DHA+Doping 17.46 80%, 17 d (air, 30% RH) [38] 2023 Air, — DHA+Doping 16.74 90%, 17 d (air, 25% RH) [39] 2023 Air, 20% RH DHA+Doping 17.39 84%, 9 d (N2, 85 ℃) [19] 2023 Air, — Doping 17.38 90%, 42 d (air, 25% RH) [40] 2023 Air, — DHA+Doping 17.40 87.25%, 30 d (air, 14% RH) [41] 2024 Air, >60% RH DHR 17.55 96%, 40 d (air, >60% RH) This work -
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