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Tuning Photocatalytic Activity in Porphyrin-Based Metal-Organic Frameworks by Controlling Charge Recombination

Tra Phuong Trinh1, Hyun Seok Lee2, Gajendra Gupta1,3

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We enhanced metal-organic frameworks (MOFs) for photocatalysis by adding phenyl-C61-butyric acid (PCBA). The free-base MOF showed superior performance due to a longer-lived charge-transfer state, unlike metalated versions.

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Area of Science:

  • Materials Science
  • Photocatalysis
  • Nanotechnology

Background:

  • Porphyrin-based metal-organic frameworks (MOFs) are effective photocatalysts.
  • Charge recombination limits the efficiency of these MOFs.
  • Incorporating electron acceptors can improve photocatalytic activity.

Purpose of the Study:

  • To enhance the photocatalytic performance of porphyrin-based MOFs.
  • To investigate the effect of incorporating phenyl-C61-butyric acid (PCBA) as an electron acceptor.
  • To understand the role of the porphyrin core's electronic nature in photocatalysis.

Main Methods:

  • Solvent-assisted ligand incorporation (SALI) method used to integrate PCBA into PCN-222 MOFs.
  • Synthesis of free-base and metalated (Co, Ni, Cu) PCBA@PCN-222 composites.
  • Photocatalytic oxidation of thioanisole under aerobic conditions.
  • Electrochemical analysis and picosecond time-resolved photoluminescence (TRPL) studies.

Main Results:

  • The free-base PCBA@PCN-222(H2) composite achieved >99% thioanisole conversion, significantly outperforming metalated analogues.
  • Metalated PCBA@PCN-222(Cu), PCBA@PCN-222(Ni), and PCBA@PCN-222(Co) showed lower conversions (23%, 3%, and 2%, respectively).
  • TRPL studies revealed a long-lived charge-transfer (CT) state (1.72 ns) in the free-base system, crucial for high activity.
  • Metal-associated quenching and ultrafast charge recombination (70-100 ps) limited the efficiency of metalated MOFs.

Conclusions:

  • The electronic nature of the porphyrin core is critical for designing efficient donor-acceptor photocatalysts.
  • Longer charge-transfer state lifetimes correlate directly with enhanced photocatalytic performance.
  • PCBA@PCN-222(H2) represents a highly efficient photocatalyst for aerobic oxidation reactions.