Biomimetic oxygen activation and electron transfer mechanism for oxidative desulfurization

• Published in: Applied catalysis. B, Environmental Environmental, 2020-10, Vol.275, p.119134, Article 119134
• Main Authors: Chi, Mingyue, Su, Ting, Sun, Lulu, Zhu, Zhiguo, Liao, Weiping, Ren, Wanzhong, Zhao, Yuchao, Lü, Hongying
• Format: Article
• Language: English
• Subjects: Activation; Biomimetics; Catalytic activity; Construction; Deep eutectic solvents; Desulfurization; Desulfurizing; Electron transfer; Ionic liquids; Oxidation; Oxidation desulfurization; Oxygen; Polyoxometalate; Polyoxometallates; Pyridines; Recoverability
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2020.119134

[Display omitted] •A green aerobic oxidative desulfurization biomimetic system was designed.•The catalytic system combined high catalytic activity and stability.•Cyclic voltammetry measurements showed a 17-fold increase in current density.•The biomimetic oxygen activation and electron transfers mechanism was revealed. Construction of biomimetic catalytic systems is recognized as one of the most prospective, but is challenging approaches to achieve efficient aerobic oxidative transformations. Herein, a green aerobic oxidative desulfurization (AODS) biomimetic system was designed, which combined an Anderson polyoxometalate (POM) -based ionic liquid (IL) with deep eutectic solvent (DES). The 3-(pyridine-1-ium-1-yl) propane-1-sulfonate]3 Co(OH)6Mo6O18 {abbreviate as [PyPS]3Co(OH)6Mo6O18} combined high catalytic activity and stability with perfect synthetic availability on the desulfurization of diesel. Also, excellent recoverability showing little decrease in activity after 5 cycles has aroused the great interest. Cyclic voltammogram measurement shows conclusive evidence of oxygen activation with a 17-fold current density increase, further confirming the reduction of the aerobic oxidation reaction barrier. It revealed the biomimetic oxygen activation and synergistic electron transfers mechanism for ODS, which may provide a new insight into the construction of biomimetic system in the future.