Zheng Mouqiao, Yi Qijie, Wang Ye, Tang Wenxiang, Ma Xiaodong, Kim Youngjae
School of Chemical Engineering, Sichuan University, Chengdu 610065, China.
School of Chemical Engineering, University of Queensland, Brisbane, Queensland 4072, Australia.
Inorg Chem. 2024 Sep 9;63(36):16842-16854. doi: 10.1021/acs.inorgchem.4c02659. Epub 2024 Aug 23.
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 (CoMnNiFeAl)O ( = 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 (CoMnNiFeAl)O catalyst exhibited the best catalytic activity. At the high space velocity of 60 000 mL·g·h, 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)O catalyst and pure cobalt oxide, respectively. Meanwhile, it has the lowest apparent activation energy (46.6 KJ·mol) and the fastest reaction rate (26.976 × 10 mol·g·s at 290 °C). The improved performance of the (CoMnNiFeAl)O 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.
具有相似催化烃类燃烧氧化活性的过渡金属基氧化物备受关注。在本研究中,通过一种简单且低成本的氯化钠模板辅助溶胶 - 凝胶法制备了一类具有多孔结构的新型金属高熵氧化物(CoMnNiFeAl)O ( = 1, 2, 3, 4, 5),并将其用于丙烷的催化氧化。结果表明,钴含量对其活性有很大影响,(CoMnNiFeAl)O催化剂表现出最佳的催化活性。在60 000 mL·g·h的高空速下,经过高温处理的优化催化剂在309 °C时仍能实现90%的丙烷转化率,分别比(CoMnNiFeAl)O催化剂和纯氧化钴低68和178 °C。同时,它具有最低的表观活化能(46.6 KJ·mol)和最快的反应速率(290 °C时为26.976 × 10 mol·g·s)。(CoMnNiFeAl)O催化剂性能的提升可归因于低温还原性的增强、活性表面氧物种数量的增加以及高熵氧化物的协同效应。这项工作为高效轻质烷烃降解催化剂的制备提供了新的见解,并为高熵氧化物在氧化催化剂领域的大规模应用提供了一种切实可行的方法。