Engineering Oxygen Vacancies of Co–Mn–Ni–Fe–Al High-Entropy Spinel Oxides by Adjusting Co Content for Enhanced Catalytic Combustion of Propane

Abstract

Transition metal-based oxides with similar oxidation activities for catalytic hydrocarbon combustion have attracted much attention. In this study, a new class of metal high-entropy oxides (Co x MnNiFeAl) 3 O 4 (x = 1, 2, 3, 4, 5) with a porous structure was fabricated through a simple and inexpensive NaCl template-assisted sol−gel approach, which was employed for the catalytic oxidation of propane. The results indicated that the content of cobalt has a great impact on its activity, and the (Co 4 MnNiFeAl) 3 O 4 catalyst exhibited the best catalytic activity. At the high space velocity of 60 000 mL•g −1 •h −1 , the optimized one with high-temperature treatment can still achieve 90% propane conversion at 309 °C, which is 68 and 178 °C lower than those of the (CoMnNiFeAl) 3 O 4 catalyst and pure cobalt oxide, respectively. Meanwhile, it has the lowest apparent activation energy (46.6 KJ•mol −1 ) and the fastest reaction rate (26.976 × 10 −6 mol•g cat −1•s −1 at 290 °C). The improved performance of the (Co 4 MnNiFeAl) 3 O 4 catalyst could be attributed to the enhancement of low-temperature reducibility, the increased number of reactive surface oxygen species, and the cocktail effect of the high-entropy oxides. This work provides new insights into the preparation of efficient light alkane degradation catalysts and a realistic approach for the large-scale application of high-entropy oxides in the field of oxidation catalysts.