An effective Mn-Co mixed oxide catalyst for the solvent-free selective oxidation of cyclohexane with molecular oxygen

An effective Mn-Co mixed oxide catalyst for the solvent-free selective oxidation of cyclohexane with molecular oxygen
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一种有效的锰钴混合氧化物催化剂,用于环己烷与分子氧的无溶剂选择性氧化

DOI:
10.1016/j.apcata.2016.06.001
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发表时间:
2016-08
期刊:
Applied Catalysis A: General
影响因子:
--
通讯作者:
Lu Guanzhong
Lu Guanzhong
中科院分区:
其他
文献类型:
--
作者:
Wu Mingzhou;Zhan Wangcheng;Guo Yanglong;Guo Yun;Wang Yunsong;Wang Li;Lu Guanzhong

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采用沉淀法制备了Mn-Co复合氧化物(MnaCobOx)催化剂,考察了Mn/Co(原子比)对Mn-Co复合氧化物催化剂结构和环己烷无溶剂选择氧化反应性能的影响。结果表明,Mn/Co原子比对MnaCoOx催化剂的相组成、比表面积、表面Mn的价态及还原性均有影响。当Mn/Co原子比为0.6时,Mn_2Co_3 O_x催化剂表现出良好的催化活性和稳定性,这主要归因于其高的比表面积和表面高的(Mn ~(4+)+Mn ~(3+))/Mn和Co ~(3+)/Co原子比。考察了Mn_2Co_3O_x催化剂的制备条件和反应条件对环己烷在Mn_2Co_3O_x催化剂上选择氧化反应的影响。在0.5 MPa O2和140 °C反应4 h的条件下,环己烷的转化率为10.4%,环己酮和环己醇混合物(KA油)的选择性为62.0%。该催化剂重复使用10次后,环己烷转化率和KA油选择性几乎没有变化。
Mn-Co mixed oxide (MnaCobOx) catalysts were prepared by the precipitation method, and the effect of Mn/Co (atom) on their structural and catalytic performance for the solvent-free selective oxidation of cyclohexane with oxygen was investigated. The results showed that the atomic ratio of Mn/Co would affect the phase constitution, surface area, surface Mn valence states and the reducibility of the MnaCobOxcatalysts. When the atomic ratio of Mn/Co in the catalyst is 0.6, the Mn2Co3Oxcatalyst behaved with excellent catalytic activity and stability, which should be attributed to its high specific surface area and the high atomic ratios of (Mn4++ Mn3+)/Mn and Co3+/Co on its surface. The effects of the preparation conditions for the Mn2Co3Oxcatalyst and the reaction conditions on the selective oxidation of cyclohexane over the Mn2Co3Oxcatalyst was tested. Under the reaction conditions of 0.5 MPa O2and 140 °C for 4 h, 10.4% conversion of cyclohexane and 62.0% selectivity to a mixture of cyclohexanone and cyclohexanol (KA oil) were achieved. After this Mn2Co3Oxcatalyst was repeatedly used 10 times, the cyclohexane conversion and the selectivity to KA oil had hardly changed.
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