Broad-Spectrum Absorption and Microsecond Excited State in Copper-MOFs for Boosting Organic Photosynthesis

The development of photosensitizing materials synergizing broad-spectrum harvesting with long-lived excited states is pivotal for advancing artificial photosynthesis. Herein, we propose a precoordination-induced coassembly strategy to integrate complementary chromophores into unsaturated Cu-MOFs (Cu-0 - Cu-123), enabling synergistic tuning of their photon absorption channels and excited states. The cosensitized Cu-123 exhibits panchromatic absorption across 200-700 nm and a prolonged excited-state lifetime of 10.2 μs via a "ping-pong" cascade energy transfer, which is over 200-fold longer than that in the pristine framework of Cu-0 (<0.05 μs). Remarkably, it achieves an outstanding yield (76.4%) in artemisinin photosynthesis and demonstrates exceptional versatility across a diverse range of organic transformations (>10 distinct reactions). Gram-scale synthesis under sunlight achieved via the construction of a continuous-flow photoreactor indicates its potential for scalable solar energy conversion. This work not only presents highly efficient photocatalysts but also establishes a general method for constructing porous photosynthesis systems with tailored photophysical properties for solar-to-chemical conversion.