Engineering oxygen vacancies in acid-etched MgMn2O4 for efficiently catalytic benzene combustion: Synergistic activation of gaseous oxygen and surface lattice oxygen

J Hazard Mater. 2024 Dec 18:486:136907. doi: 10.1016/j.jhazmat.2024.136907. Online ahead of print.

Abstract

The synergistic activation of gaseous oxygen and surface lattice oxygen is essential for designing highly efficient catalysts to eliminate VOCs. Herein, an effective acid treatment was carried out to create more oxygen vacancies by modulating the electronic structure of MgMn2O4 spinels and MgMnOx mixed oxides. The acid-treated MgMn2O4 exhibited outstanding catalytic performance, with the reaction rate of benzene rising by 8.55 times at 200 °C. After acid treatment, MgMn2O4 partially retained its spinel structure, while Mn2O3 in situ grew on the surface due to the selective removal of Mg2+. The transformation of Mn-O-Mg into Mn-O weakened the strength of adjacent Mn-O bonds, thereby promoting the release of surface lattice oxygen and the regeneration of oxygen vacancies. In addition, acid-treated MgMn2O4 facilitated the adsorption and activation of gaseous oxygen. In situ DRIFTS analysis proved that the synergistic activation of gaseous oxygen and surface lattice oxygen accelerated the conversion of intermediates, thus contributing to the efficient degradation of benzene.

Keywords: Acid treatment; Benzene oxidation; Oxygen species; Oxygen vacancies; Spinel catalyst.