Journal
APPLIED CATALYSIS A-GENERAL
Volume 590, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcata.2019.117340
Keywords
Heterogeneous catalysis; MIL-101(Cr)-NO(2)as catalyst; Aerobic oxidations; Thiophenol coupling; Fuel; Desulfurization
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Funding
- Spanish Ministry of Science and Innovation [RTI2018-098237-CO21]
- Generalitat Valenciana [Prometeo 2017/083]
- Fundacion Ramon Areces (XVIII Concurso Nacional para la Adjudicacion de Ayudas a la Investigacion en Ciencias de la Vida y de la Materia, 2016)
- Ministerio de Ciencia, Innovacion y Universidades [CTQ-2018 RTI2018-099482-A-I00]
- Generalitat Valenciana grupos de investigacion consolidables 2019 [AICO2019/214]
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A series of MIL-101(Cr)-X functionalized with electron withdrawing (NO2, SO3H or Cl) or electron donor (NH2 or CH3) groups has been tested for the solvent-free oxidative coupling of thiophenol to disulfides. No byproducts were observed. A relationship between the catalytic activity of these MOFs with the substituent meta Hammet constant on the terephthalate ligand and with their redox potential was found, MIL-101(Cr)-NO2 being the most active catalyst. NO2-substituted MIL-101 is also more efficient than the parent MIL-101(Cr) to promote the aerobic desulfurization of dibenzothiophenes in n-dodecane or commercial Diesel as solvent. No byproduct formation was observed. Mechanistic studies reveal that MIL-101(Cr)-NO2 is acting as heterogeneous catalyst in thiophenol oxidation and as radical initiator for the aerobic desulfurization. For both reactions, the catalyst can be reused without deactivation, maintaining its crystallinity and with negligible metal leaching.
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