As a leading contender to replace lead halide perovskites, tin‐based perovskites have demonstrated ever increasing performance in solar cells and light‐emitting diodes (LEDs). They tend to be processed with dimethyl sulfoxide (DMSO) solvent, which has been identified as a major contributor to the Sn(II) oxidation during film fabrication, posing a challenge to the further improvement of Sn‐based perovskites. Herein, we use NMR spectroscopy to investigate the kinetics of the oxidation of SnI2, revealing that autoamplification takes place, accelerating the oxidation as the reaction progresses. We propose a mechanism consistent with these observations involving water participation and HI generation. Building upon these insights, we have developed low‐temperature Sn‐based perovskite LEDs (PeLEDs) processed at 60 °C, achieving enhanced external quantum efficiencies (EQEs). Our research underscores the substantial potential of low‐temperature DMSO solvent processes and DMSO‐free solvent systems for fabricating oxidation‐free Sn‐based perovskites, shaping the future direction in processing Sn‐containing perovskite materials and optoelectronic devices.

中文翻译：

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控制钙钛矿光电器件溶液中卤化锡钙钛矿氧化动力学


作为取代卤化铅钙钛矿的主要竞争者，锡基钙钛矿已在太阳能电池和发光二极管（LED）中表现出不断增强的性能。它们往往用二甲基亚砜（DMSO）溶剂进行处理，该溶剂已被认为是薄膜制造过程中 Sn(II) 氧化的主要贡献者，这对锡基钙钛矿的进一步改进提出了挑战。在这里，我们使用核磁共振波谱研究了 SnI2 氧化的动力学，揭示了自动放大的发生，随着反应的进行加速了氧化。我们提出了一种与这些涉及水参与和 HI 生成的观察相一致的机制。基于这些见解，我们开发了在 60 °C 下加工的低温锡基钙钛矿 LED (PeLED)，实现了增强的外部量子效率 (EQE)。我们的研究强调了低温 DMSO 溶剂工艺和无 DMSO 溶剂系统在制造无氧化锡基钙钛矿方面的巨大潜力，塑造了含锡钙钛矿材料和光电器件加工的未来方向。