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

Area of Science:

• Materials Science
• Photochemistry
• Catalysis

Background:

• Artificial photosynthesis requires efficient photosensitizers with broad light absorption and long-lived excited states.
• Developing integrated systems that synergistically combine light harvesting and charge separation is crucial.

Purpose of the Study:

• To design and synthesize novel unsaturated copper metal-organic frameworks (Cu-MOFs) for enhanced artificial photosynthesis.
• To achieve synergistic tuning of photon absorption and excited-state properties through chromophore coassembly.

Main Methods:

• A precoordination-induced coassembly strategy was employed to integrate complementary chromophores into unsaturated Cu-MOFs.
• Characterization of photophysical properties including absorption spectra and excited-state lifetimes.
• Evaluation of photocatalytic performance in artemisinin photosynthesis and diverse organic transformations.

Main Results:

• The cosensitized Cu-123 exhibited panchromatic absorption (200-700 nm) and a significantly prolonged excited-state lifetime (10.2 μs).
• Achieved an outstanding yield (76.4%) in artemisinin photosynthesis and demonstrated versatility in over 10 organic reactions.
• Gram-scale synthesis was achieved using a continuous-flow photoreactor under sunlight, indicating scalability.

Conclusions:

• The developed Cu-MOFs serve as highly efficient photocatalysts for solar-to-chemical conversion.
• The precoordination coassembly strategy provides a general method for constructing porous photosynthesis systems with tailored photophysical properties.
• This approach holds potential for scalable solar energy conversion applications.