Halide segregation critically limits the stability of mixed-halide perovskite solar cells under device operational conditions. There is a strong indication that halide oxidation is the primary driving force behind halide de-mixing. To alleviate this problem, we develop a series of multifunctional redox mediators based on anthraquinone that selectively reduce iodine and oxidize metallic Pb⁰, while simultaneously passivating defects through tailored cationic substitution. These effects enable wide-bandgap perovskite solar cells to achieve a power conversion efficiency of 19.58% and a high open-circuit voltage of 1.35 V for 1.81-eV PSCs. The device retains 95% of its initial efficiency after operating at its maximum power point for 500 h. Most notably, by integrating the perovskite device into the monolithic perovskite-organic tandem solar cell as a wide-bandgap subcell, we report an efficiency of 25.22% (certified 24.27%) with impressive long-term operational stability (T₉₀ > 500 h).

卤化物偏析严重限制了混合卤化物钙钛矿太阳能电池在器件运行条件下的稳定性。有强烈的迹象表明卤化物氧化是卤化物分层的主要驱动力。为了缓解这个问题，我们开发了一系列基于蒽醌的多功能氧化还原介体，可以选择性地还原碘并氧化金属Pb ⁰，同时通过定制的阳离子取代来钝化缺陷。这些效应使宽带隙钙钛矿太阳能电池能够实现 19.58% 的功率转换效率和 1.81-eV PSC 的 1.35 V 高开路电压。该器件在最大功率点运行 500 小时后仍保留 95% 的初始效率。最值得注意的是，通过将钙钛矿器件作为宽带隙子电池集成到单片钙钛矿-有机串联太阳能电池中，我们报告效率为 25.22%（认证为 24.27%），并且具有令人印象深刻的长期运行稳定性（T ₉₀  > 500 小时） 。