Enabling green-solvent-processed large-area organic solar cells (OSCs) is of great significance to their industrialization. However, precisely controlling the temperature-dependent fluid mechanics and evaporation behavior of green solvents with high-boiling points is challenging. Controlling these parameters is essential to prevent the non-uniform distribution of active layer components and severe molecule aggregation, which collectively degrade the power conversion efficiency (PCE) of large-scale devices. In this study, we revealed that the temperature gradient distribution across a wet film is the root of the notorious Marangoni effect, which leads to the formation of a severely non-uniform active layer on a large scale. Thus, a rapid solidification strategy was proposed to accelerate the evaporation of toluene, a green solvent, at room temperature. This strategy simultaneously inhibits the Marangoni effect and suppresses molecular aggregation in the wet film, allowing the formation of a nano-scale phase separation active layer with uniform morphology. The resultant toluene-processed 15.64-cm² large-area OSC module achieves an outstanding PCE of 16.03% (certified: 15.69%), which represents the highest reported PCE of green-solvent-processed OSC modules. Notably, this strategy also exhibits a weak scale dependence on the PCE, and we successfully achieved a state-of-the-art PCE of 14.45% for a 72.00-cm² OSC module.

中文翻译：

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绿色溶剂加工大面积有机太阳能电池组件的快速固化，效率 >16%

实现绿色溶剂加工的大面积有机太阳能电池（OSC）对其产业化具有重要意义。然而，精确控制高沸点绿色溶剂的温度依赖性流体力学和蒸发行为具有挑战性。控制这些参数对于防止有源层成分的不均匀分布和严重的分子聚集至关重要，这会共同降低大型器件的功率转换效率（PCE）。在这项研究中，我们发现湿膜上的温度梯度分布是臭名昭著的马兰戈尼效应的根源，该效应导致大规模形成严重不均匀的活性层。因此，提出了一种快速固化策略来加速绿色溶剂甲苯在室温下的蒸发。该策略同时抑制马兰戈尼效应并抑制湿膜中的分子聚集，从而形成具有均匀形态的纳米级相分离活性层。由此产生的甲苯处理的15.64-cm ²大面积OSC模块实现了16.03%的出色PCE（认证：15.69%），这是报道的绿色溶剂处理OSC模块的最高PCE。值得注意的是，该策略还表现出对 PCE 的弱规模依赖性，我们成功地为 72.00-cm ² OSC 模块实现了 14.45% 的最先进 PCE 。