1. Partial Metalation of Porphyrin Moieties in Hydrogen‐Bonded Organic Frameworks Provides Enhanced CO2 Photoreduction Activity.
- Author
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Zhang, An‐An, Si, Duanhui, Huang, Haibo, Xie, Lei, Fang, Zhi‐Bin, Liu, Tian‐Fu, and Cao, Rong
- Subjects
METALATION ,PORPHYRINS ,MOIETIES (Chemistry) ,PHOTOREDUCTION ,CATALYTIC activity ,HETEROGENEOUS catalysts - Abstract
In natural photosynthesis, the architecture of multiproteins integrates more chromophores than redox centers and simultaneously creates a well‐controlled environment around the active site. Herein, we demonstrate that these features can be emulated in a prototype hydrogen‐bonded organic framework (HOF) through simply varying the proportion of metalated porphyrin in the structure. Further studies demonstrate that changing the metalloporphyrin content not only realizes a fine tuning of the photosensitizer/catalyst ratio, but also alters the microenvironment surrounding the active site and the charge separation efficiency. As a result, the obtained material achieves the challenging overall CO2 reduction with a high HCOOH production rate (29.8 μmol g−1 h−1, scavenger free), standing out from existing competitors. This work unveils that the degree of metalation is vital to the catalytic activity of the porphryinic framework, presenting as a new strategy to optimize the performance of heterogeneous catalysts. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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