【摘要】 钙钛矿太阳能电池因其优异的光电性能而受到广泛关注，但其稳定性不足仍制约着实际应用。本文提出一种基于二维/三维（2D/3D）异质结构的协同钝化策略，通过碘代-4氨基-TEMPO诱导形成的2D钙钛矿表面层与稳定自由基的复合调控，实现了晶界缺陷与自由基诱导降解的双重抑制。结果表明，该策略显著改善了钙钛矿薄膜的结晶质量与表面平整度，AFM测得表面粗糙度（RMS）由9.60 nm降至6.25 nm；稳态与瞬态光致发光结果显示，载流子寿命由250 ns延长至355 ns，非辐射复合明显抑制。基于2D/3D异质结的器件表现出更高的复合电阻（383.7Ω）与优异的电荷传输特性，获得最高光电转换效率21.15%。同时，器件在湿热环境下20天后仍保留初始效率的71.5%。该研究为实现高效率与高稳定性兼顾的钙钛矿光伏器件提供了新的设计思路与材料策略。更多还原

【Abstract】 Perovskite solar cells(PSCs) show great promise owing to their remarkable optoelectronic performance, yet their commercial deployment is hindered by intrinsic instability. We introduce a synergistic 2D/3D heterostructure passivation approach, integrating a TAI-derived 2D perovskite capping layer with the TEMPO radical scavenger to concurrently mitigate grain boundary defects and radical-induced degradation. This strategy improves perovskite crystallinity and film uniformity, lowering the surface roughness from 9. 60 nm to 6. 25 nm. Carrier lifetime extends from 250 ns to 355 ns, as confirmed by steady-state and time-resolved photoluminescence, indicating suppressed non-radiative recombination. The 2D/3D-based devices demonstrate enhanced recombination resistance(383. 7 Ω) and superior charge transport, yielding a champion efficiency of 21. 15%. The device retained 71. 5% of its initial efficiency after 20 days in a damp-heat environment. This study offers a new materials design paradigm toward efficient and operationally stable perovskite photovoltaics.更多还原