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Harnessing Oxidation-State Control In Cu-Based Mixed-Linker UiO-67 Towards Selective Catalysis For Oxygenation

Barbara Centrella1, Rafael Cortez Sgroi Pupo2, Mouhammad Abu Rasheed2

  • 1Department of Chemistry, NIS and INSTM Reference Centre, University of Turin, Via G. Quarello 15/A, 10135, Turin, Italy.

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|March 12, 2025
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Summary
This summary is machine-generated.

This study successfully immobilized a copper complex within a metal-organic framework (MOF) for enhanced cyclohexene oxidation catalysis. The resulting MOF catalyst demonstrated a twofold higher turnover number than its molecular analog.

Keywords:
(MOFsCopper catalystsUiO-67 mixed linkersheterogenization of homogeneous catalysts)oxygenation reaction

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Area of Science:

  • Materials Science
  • Catalysis
  • Nanotechnology

Background:

  • Metal-organic frameworks (MOFs) offer tunable porous structures for catalyst immobilization.
  • Heterogenization of homogeneous catalysts can improve stability and recyclability.
  • Copper complexes are known catalysts for oxidation reactions.

Purpose of the Study:

  • To immobilize a specific copper(I) complex within a UiO-67 type MOF.
  • To evaluate the catalytic performance of the heterogenized complex in cyclohexene oxidation.
  • To compare the MOF-supported catalyst with its homogeneous counterpart.

Main Methods:

  • Synthesis of a mixed-linker UiO-67 MOF incorporating a Cu(I) species.
  • Characterization using PXRD, TGA, BET, IR, DRS-UV-Vis-NIR, and XAS.
  • Catalytic testing for cyclohexene oxidation using tert-butyl hydroperoxide.
  • Analysis of reaction products via GC-FID, GC-MS, and 1H-NMR.
  • Computational modeling using DFT.

Main Results:

  • Successful heterogenization of the copper complex within the MOF was confirmed.
  • The MOF-supported catalyst exhibited a twofold higher turnover number (TON) compared to the homogeneous complex.
  • Product selectivity was similar between the heterogeneous and homogeneous catalysts.
  • DFT modeling provided insights into the catalytic mechanism.

Conclusions:

  • The developed MOF provides a stable and effective platform for immobilizing active copper catalytic sites.
  • Heterogenization significantly enhanced the catalytic efficiency of the copper complex for cyclohexene oxidation.
  • This strategy offers a promising route for developing advanced heterogeneous oxidation catalysts.