Ce-based three-dimensional mesoporous microspheres with Mn homogeneous incorporation for toluene oxidation.

J Colloid Interface Sci

College of New Energy, China University of Petroleum (East China), 66 West Changjiang Road, Qingdao 266580, China; Qingdao Engineering Research Center of Efficient and Clean Utilization of Fossil Energy, Qingdao 266580, China.

Published: September 2024

Ce-based three-dimensional (3D) mesoporous microspheres with Mn homogeneous incorporation were synthesized. The CeMn-0.4, characterized by a Ce/Mn molar ratio of 6:4, demonstrated exceptional catalytic activity and stability. The formation of CeMn solid solution strengthened the Ce-Mn interaction, yielding higher concentrations of Ce and Mn. Mn initiated toluene preliminary activation owing to its robust oxidative properties, while Ce contributed to oxygen vacancy generation, enhancing the activation of gaseous oxygen and lattice oxygen mobility. Integrating experiments and Density Functional Theory (DFT) calculations elucidated the oxygen reaction mechanisms. A portion of oxygen was converted into surface reactive oxygen species (O) that directly oxidized toluene. Additionally, the presence of oxygen vacancies promoted the participation of oxygen in toluene oxidation by converting it into lattice oxygen, which was crucial for the deep oxidation of toluene. Diffuse Reflectance Fourier Transform Infrared Spectroscopy (DRIFTS) indicated the accumulation of benzene-ring intermediates on the catalyst surface hindered continuous toluene oxidation. Thus, the abundant oxygen vacancies in CeMn-0.4 played a pivotal role in sustaining the oxidation process by bolstering the activation of gaseous oxygen and the mobility of lattice oxygen.

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http://dx.doi.org/10.1016/j.jcis.2024.04.128DOI Listing

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