Sphere-Shaped Mn3O4 Catalyst with Remarkable Low-Temperature Activity for Methyl-Ethyl-Ketone Combustion

Sphere-Shaped Mn3O4 Catalyst with Remarkable Low-Temperature Activity for Methyl-Ethyl-Ketone Combustion
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DOI:
10.1021/acs.est.7b00136
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发表时间:
2017-06-06
影响因子:
11.4
通讯作者:
Liu, Hongxia
Liu, Hongxia
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Pan, Hua;Jian, Yanfei;Liu, Hongxia

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采用溶剂热法合成了Mn 3 O 4、FeMnOx和FeOx催化剂,并将其用于甲乙酮(MEK)的低温催化氧化。具有球形形貌的Mn 3 O 4对MEK氧化表现出最高的活性,在200 ℃下,MEK被完全氧化为CO2,并且该结果可以与典型的贵金属负载催化剂相媲美。MEK在Mn_3O_4上的活化能(30.8 kJ/mol)远低于FeMnOx(41.5 kJ/mol)和FeOx(47.8 kJ/mol)。催化剂的优势晶面、表面锰物种比、表面吸附氧和氧化还原能力对催化剂的催化活性起着重要作用,而比表面积与MEK去除率之间没有明显的相关性。Mn_3O_4活性最高,其主要原因是氧空位多,表面Mn ~(4+)含量低,还原性强。在Mn_3O_4催化剂上,甲乙酮经中间体丁二酮氧化为CO_2是一条反应途径。球形Mn_3O_4具有高效、低成本等优点,是一种很有前途的VOCs治理催化剂。
Mn3O4, FeMnOx, and FeOx catalysts synthesized via a solvothermal method were employed for catalytic oxidation of methyl-ethyl-ketone (MEK) at low temperature. Mn3O4 with sphere-like morphology exhibited the highest activity for MEK oxidation, over which MEK was completely oxidized to CO2 at 200 degrees C, and this result can be comparable to typical noble metal loaded catalysts. The activation energy of MEK over Mn3O4 (30.8 kJ/mol) was much lower than that of FeMnOx (41.5 kJ/mol) and FeOx (47.8 kJ/mol). The dominant planes, surface manganese species ratio, surface-absorbed oxygen, and redox capability played important roles in the catalytic activities of catalysts, while no significant correlation was found between specific surface area and MEK removal efficiency. Mn3O4 showed the highest activity, accounting for abundant oxygen vacancies, low content of surface Mn4+ and strong reducibility. The oxidation of MEK to CO2 via an intermediate of diacetyl is a reaction pathway on Mn3O4 catalyst. Due to high efficiency and low cost, sphere-shaped Mn3O4 is a promising catalyst for VOCs abatement.