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[UiO-68-BT] Blue light-driven selective aerobic oxidation of amines by benzothiadiazole MOFs photocatalysis
Summary:
The authors from Wuhan University developed a benzothiadiazole metal–organic framework (MOF) photocatalyst UiO-68-BT, achieving high conversion and selectivity in blue light-driven selective aerobic oxidation of amines.
Background:
1. To address the problem of low efficiency and poor selectivity in photocatalytic oxidation reactions, previous researchers have explored various MOFs as photocatalysts, achieving some success. However, challenges remain in enhancing the charge separation and transfer efficiency of MOFs.
2. The authors in this work proposed an innovative method by tuning the electron-withdrawing effect of organic ligands in Zr-based MOFs, obtaining superior photocatalytic performance.
Research Content:
1. Synthesis:
The authors synthesized UiO-68-BT and UiO-68-NH2 using the solvothermal method with Zr6O4(OH)412+ clusters and linear dicarboxylic ligands.
2. Characterizations:
1) BET surface areas were 405 m² g⁻¹ for UiO-68-BT and 107 m² g⁻¹ for UiO-68-NH2. Pore size distributions were centered on 2.49 nm for UiO-68-BT and 2.24 nm for UiO-68-NH2.
2) SEM/TEM tests show the particle size of UiO-68-BT with an octahedral shape and high crystallinity.
3) Electrochemical and photoelectrochemical measurements revealed that UiO-68-BT exhibited higher photocurrent density and more efficient charge separation than UiO-68-NH2.
3. Application:
UiO-68-BT achieved a conversion of 93% and selectivity of 99% in the blue light-driven selective aerobic oxidation of benzylamine within 45 min. It also demonstrated excellent recyclability.
4. Mechanism:
The analysis of the experimental results indicated that the benzothiadiazole unit in the ligand significantly enhanced charge separation and transfer efficiency. The generation of superoxide radical anion (O2˙−) played a pivotal role in the selective oxidation process.
Outlook:
This research highlights the benefits of modulating the electronic effect of organic ligands in MOF photocatalysts, offering a new avenue for designing highly efficient photocatalysts for aerobic oxidation reactions.
Blue light-driven selective aerobic oxidation of amines by benzothiadiazole metal–organic framework photocatalysis
Authors: Bing Zeng, Yuexin Wang, Fengwei Huang, Kanghui Xiong, Keke Zhang, Xianjun Lang
DOI: 10.1039/d4cy00312h
Link: https://doi.org/10.1039/d4cy00312h
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