Dual-fixations of europium cations and TEMPO species on metal-organic frameworks for the aerobic oxidation of alcohols

Seongwoo Kim, Jooyeon Lee, Sungeun Jeoung, Hoi Ri Moon, Min Kim

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The efficient and selective aerobic oxidation of alcohols has been investigated with judicious combinations of europium-incorporated and/or TEMPO ((2,2,6,6-tetramethylpiperidin-1-yl)oxyl)-functionalized zirconium-based porous metal-organic frameworks (MOFs). Although MOFs are well-known catalytic platforms for the aerobic oxidation with radical-functionalities and metal nanoparticles, these systematic approaches involving metal cations and/or radical species introduce numerous interesting aspects for cooperation between metals and TEMPO for the aerobic oxidation of alcohols. The role of TEMPO as the oxidant in the heterogeneous catalytic aerobic oxidation of alcohols was revealed through a series of comparisons between metal-anchored, TEMPO-anchored, and metal and TEMPO-anchored MOF catalysis. The fine tunability of the MOF allowed the homogeneously and doubly functionalized catalysts to undergo organic reactions in the heterogeneous media. In addition, the well-defined and carefully designed heterogeneous molecular catalysts displayed reusability along with better catalytic performance than the homogeneous systems using identical coordinating ligands. The role of metal-cation fixation should be carefully revised to control their coordination and maximize their catalytic activity. Lastly, the metal cation-fixed MOF displayed better substrate tolerance and reaction efficiencies than the TEMPO-anchored MOF or mixture MOF systems.

Original languageEnglish
Pages (from-to)8060-8066
Number of pages7
JournalDalton Transactions
Issue number24
StatePublished - 28 Jun 2020

Bibliographical note

Funding Information:
We thank Mr Chan Hee Ryu and Prof. Dr Kang Mun Lee (Kangwon National University, Korea) for experimental help and discussions. This work was supported by the Basic Science Research Program (2019R1A2C4070584) and the Science Research Center (2016R1A5A1009405) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, and ICT. S. Kim and J. Lee were supported by the NRF Global Ph.D. Fellowship program (2018H1A2A1062013 for S. Kim; 2019H1A2A1076014 for J. Lee) funded by the Ministry of Education.

Publisher Copyright:
This journal is © The Royal Society of Chemistry.


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