Inspired by nature, improving photosensitization represents a vital direction for the development of artificial photosynthesis. The sensitization ability of photosensitizers (PSs) reflects in their electron-transfer ability, which highly depends on their excited-state lifetime and redox potential. Herein, for the first time, we put forward a facile strategy to improve sensitizing ability via finely tuning the excited state of Ru(II)-PSs (Ru-1–Ru-4) for efficient CO₂ reduction. Remarkably, [Ru(Phen)₂(3-pyrenylPhen)]²⁺ (Ru-3) exhibits the best sensitizing ability among Ru-1–Ru-4, over 17 times higher than that of typical Ru(Phen)₃²⁺. It can efficiently sensitize a dinuclear cobalt catalyst for CO₂-to-CO conversion with a maximum turnover number of 66 480. Systematic investigations demonstrate that its long-lived excited state and suitable redox driving force greatly contributed to this superior sensitizing ability. This work provides a new insight into dramatically boosting photocatalytic CO₂ reduction via improving photosensitization.

中文翻译：

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提高光化学 CO2 到 CO 转化的光敏性

受自然启发，提高光敏性是人工光合作用发展的重要方向。光敏剂（PSs）的敏化能力反映在它们的电子转移能力上，这在很大程度上取决于它们的激发态寿命和氧化还原电位。在此，我们首次提出了一种通过微调 Ru(II)-PSs ( Ru-1 – Ru-4 )的激发态来提高敏化能力的简便策略，以有效还原CO ₂。值得注意的是，[Ru(Phen) ₂ (3-pyrenylPhen)] ²⁺ ( Ru-3 ) 在Ru-1 – Ru-4 中表现出最好的敏化能力，比典型的 Ru(Phen) 高 17 倍以上₃ ²⁺。它可以有效地敏化双核钴催化剂，用于 CO ₂到 CO 的转化，最大转换数为 66 480。系统研究表明，其长寿命的激发态和合适的氧化还原驱动力极大地促进了这种卓越的敏化能力。这项工作为通过改善光敏化显着促进光催化 CO ₂还原提供了新的见解。