"Two‐in‐One" Strategy of o‐Amino and Aromatic Nitrogen in Biomimetic Metal‐Organic Frameworks for Efficient CO2 Photoconversion

Visible‐light driven photoconversion of CO2 into energy carriers is highly important to the natural carbon balance and sustainable development. Herein, we demonstrate the biological nucleobase adenine‐dependent CO2 photoreduction performance in green biomimetic metal‐organic frameworks. Photocatalytic results indicate that AD‐MOF‐2 exhibited a very high HCOOH production rate of 443.2 μmol g‐1 h‐1 in pure aqueous solution, which is more than two times higher than that of AD‐MOF‐1 (179.0 μmol hour−1 g−1) in acetonitrile solution. Significantly, experimental and theoretical evidences reveal that CO2 photoreduction reaction mainly takes place on biological adenine molecules by unique o‐amino assisted active aromatic nitrogen atom rather than traditional metal center. This work not only serves as an important case study for the development of green biomimetic photocatalysts used for artificial photosynthesis, but also proposes a new catalytic strategy for efficient CO2 photoconversion.

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