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Visible-light harvesting pyrene-based MOFs as efficient ROS generators.

Yingmu Zhang¹, Jiandong Pang¹, Jialuo Li¹

¹Department of Chemistry , Texas A&M University , College Station , Texas 77842-3012 , USA .

Chemical Science

|December 6, 2019

Summary

New porous metal-organic frameworks (MOFs) efficiently generate reactive oxygen species (ROS) using visible light. PCN-822(Hf) activates oxygen for amine oxidation, advancing green chemistry.

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Area of Science:

Materials Science
Photochemistry
Organic Synthesis

Background:

Reactive oxygen species (ROS) are valuable oxidants for mild organic transformations.
Metal-organic frameworks (MOFs) show promise as photosensitizers for ROS generation.
Visible-light responsive MOFs for oxygen activation are currently limited.

Purpose of the Study:

To design and synthesize novel porous MOFs responsive to visible light for ROS generation.
To investigate the application of these MOFs in photochemical synthesis, specifically oxygen activation.
To explore the catalytic activity of hafnium-based MOFs in organic oxidation reactions.

Main Methods:

Synthesis of two porous MOFs, PCN-822(Zr) and PCN-822(Hf), using a pyrene-based ligand (BPETB4-).
Characterization of MOF properties, including porosity and light absorption (225-650 nm).
Evaluation of MOF performance as ROS generators under visible-light irradiation and catalytic oxidation of amines to imines.

Main Results:

The synthesized MOFs, PCN-822(M), exhibit extended π-conjugation and broad visible-light absorption.
Both MOFs function as efficient ROS generators upon visible-light irradiation.
PCN-822(Hf) effectively catalyzes the oxidation of amines to imines by activating molecular oxygen via photo-induced energy and charge transfer.

Conclusions:

The developed MOFs are highly effective visible-light-driven ROS generators.
PCN-822(Hf) offers a promising catalytic system for green oxidation reactions using molecular oxygen.
This work expands the scope of MOF applications in visible-light photochemistry and sustainable synthesis.