Oxidative dehydrogenation of ethane to ethylene over NiO loaded on high surface area MgO

Oxidative dehydrogenation of ethane to ethylene over NiO loaded on high surface area MgO
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DOI:
10.1016/j.molcata.2006.06.058
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发表时间:
2006-12
影响因子:
--
通讯作者:
Kentaro Nakamura;T. Miyake;T. Konishi;Toshimitsu Suzuki
Kentaro Nakamura;T. Miyake;T. Konishi;Toshimitsu Suzuki
中科院分区:
化学2区
文献类型:
--
作者:
Kentaro Nakamura;T. Miyake;T. Konishi;Toshimitsu Suzuki

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采用固定床流动反应器,在600°C、常压下,以NiO负载的高比表面积MgO为催化剂,进行了乙烷氧化脱氢反应。在600°C下,乙烷(C2 H6/O2=1)在不用惰性气体稀释的情况下的氧化脱氢导致C2 H6转化率为68.8%和高C2 H4选择性为52.8%,这对应于C2 H4产率为36.3%。此外,催化活性在10 h内没有下降。反应后催化剂的X射线光电子能谱表明,Ni ~(2+)(NiO)在乙烷氧化脱氢反应中保持了初始价态。然而,当NiO负载的MgO在反应前用H2还原时,C2 H4选择性降低到接近零,并且在C2 H6转化率为50%的情况下观察到高的CO和H2选择性,表明C2 H6的部分氧化进行。因此,似乎重要的是保持Ni物种作为载体上的氧化物相,并且为此目的,使用MgO的高表面积是必要的。
The oxidative dehydrogenation of ethane over NiO-loaded MgO with high surface area was carried out using a fixed-bed flow reactor at 600°C under atmospheric pressure. At 600°C, the oxidative dehydrogenation of ethane (C2H6/O2=1) without dilution with an inert gas resulted in C2H6conversion of 68.8% and a high C2H4selectivity of 52.8%, which corresponds to a C2H4yield of 36.3%. In addition, the catalytic activity did not decrease for at least 10h. X-ray photoelectron spectra of the catalysts after the reaction exhibited that the initial valence state of Ni2+(NiO) was maintained during the oxidative dehydrogenation of ethane. However, when NiO-loaded MgO was reduced with H2prior to the reaction, C2H4selectivity decreased to nearly zero and high CO and H2selectivities were observed with the C2H6conversion of 50 %, indicating that partial oxidation of C2H6proceeded. Therefore, it seems important to keep Ni species as an oxide phase on the support, and for this purpose, use of the high surface area of MgO is essential.