Inspired by efficient perovskite solar cells, we developed a three-component hybrid perovskite-based solar photocatalyst cell, NiO_x/FAPbBr₃/TiO₂, for C(sp³)–H bond activation with high selectivity (∼90%) and high conversion rates (3800 μmol g^–1 h^–1) under ambient conditions. Time-resolved spectroscopy on our photocatalytic cell reveals efficient exciton dissociation and charge separation, where TiO₂ and NiO_x serve as the electron- and hole-transporting layers, respectively. The photogenerated charge carriers injected into TiO₂ and NiO_x drive the challenging C–H activation reaction via the synergetic effects of their band alignment relative to FAPbBr₃. The reaction pathway is investigated by controlling the free-radical formation, and we find that C–H activation is mainly triggered by hole oxidation. Besides aromatic alkanes, also the C(sp³)–H bond in cycloalkanes can be oxidized selectively. This work demonstrates a generic strategy for engineering high-performance photocatalysts based on the perovskite solar cell concept.

中文翻译：

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钙钛矿型太阳能光催化剂对C（sp ³）–H键的活化作用

受高效钙钛矿太阳能电池的启发，我们开发了一种三组分混合钙钛矿基太阳能光催化剂电池NiO _x / FAPbBr ₃ / TiO ₂，用于高选择性（〜90％）和高选择性的C（sp ³）–H键活化在环境条件下的转化率（3800μmolg ^–1 h ^–1）。我们的光催化电池上的时间分辨光谱显示出有效的激子解离和电荷分离，其中TiO ₂和NiO _x分别用作电子和空穴传输层。注入TiO ₂和NiO _x中的光生载流子相对于FAPbBr ₃，通过其能带排列的协同效应来驱动具有挑战性的CH活化反应。通过控制自由基的形成来研究反应途径，我们发现C–H活化主要是由空穴氧化触发的。除了芳香族烷烃外，环烷烃中的C（sp ³）–H键也可以被选择性氧化。这项工作展示了一种基于钙钛矿太阳能电池概念设计高性能光催化剂的通用策略。