期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 260, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2019.118150
关键词
Toluene oxidation; MnO2; HAADF; Oxygen vacancies; In-situ DRIFTS
资金
- National Natural Science Foundation of China [21777081]
- national key research and development program of China [2016YFE0126600, 2016YFCO209203]
The structure-performance relationship of alpha-, beta-, gamma- and delta-MnO2 catalysts were studied. The four samples exhibited different activities of toluene oxidation in terms of distinct tunnel sizes, surface-active oxygen and redox properties. delta-MnO2 catalyst with K+ in the mezzanines of its layers presented the highest toluene oxidation activity under a GHSV of 60,000 mL.g(-1) h(-1), as well as good water resistance. HAADF images and EELS results showed that oxygen vacancies preferred to form on delta-MnO2 lattice with layer stack dislocations via Mn4+ reduction rather than beta-MnO2 with good crystallization. These inherent-distorted structures with heterocations K+ improved the emerge-annihilate cycling of oxygen vacancies. In-situ DRIP IS results showed that toluene adsorption was facilitated via rapid dehydrogenation of methyl due to abundant surface adsorbed oxygen on delta-MnO2. In addition, benzoate, maleic and manganese carbonate on delta-MnO2 were the key intermediate species during toluene oxidation at relatively low temperatures.
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