Catalytic combustion of propane over Mg-modified Co1.5Mn1.5O4 spinel catalysts: Boosting C-H cleavage with Lewis acid and oxygen vacancies

Rational modulation of surface electronic structure can optimize the adsorption and activation of reactant molecules on the catalyst surface, which is crucial for catalytic elimination of hydrocarbons. Herein, a facile low-valence Mg doping strategy was applied to synthesize highly active and stable Co-Mn binary oxide (CMO) catalyst. Lewis acid sites and oxygen vacancies were purposefully introduced on CMO through the surface electron deficit caused by the substitution of doped Mg for host metals. For the CMO catalyst modified by appropriate amount of Mg (CMO-Mg0.05), the Co-Mn spinel with lattice expansion is significantly modified through substitution of Co or Mn ions with Mg2+, resulting in generation of abundant higher metal oxidation state species (Co3+, Mn4+) and oxygen vacancies. The best performance for catalytic propane combustion was achieved on CMO-Mg0.05 catalyst, with the T90 at 255 degrees C under high space velocity (60,000 ml g-1 h-1). Meanwhile, clear improvements on stability and water resistance were also achieved after the modification of Mg in CMO catalyst. Combined with C3H8-TPD, in-situ DRIFTS and various characterizations, it can be revealed that the synergistic effect of Lewis-acid sites and oxygen vacancies would remarkably promote the process of propane dissociative adsorption and mineralization. This work not only gives insight into the Mg dopants in boosting C-H activation on CMO catalyst, but also provides a potential strategy for fabricating highly active hydrocarbon combustion catalysts.

Automated summary

Rational modulation of surface electronic structure through low-valence Mg doping strategy enhances the activity and stability of Co-Mn binary oxide (CMO) catalyst for hydrocarbon combustion. The introduction of Lewis acid sites and oxygen vacancies promotes the process of propane dissociative adsorption and mineralization. This work provides insight into the role of Mg dopants in boosting C-H activation and offers a potential strategy for fabricating highly active hydrocarbon combustion catalysts.