Ethylene oligomerization into linear olefins over cobalt oxide on carbon catalyst

Ethylene oligomerization into linear olefins over cobalt oxide on carbon catalyst
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氧化钴碳催化剂上乙烯齐聚成直链烯烃

DOI:
10.1039/d1cy00207d
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发表时间:
2021
影响因子:
5
通讯作者:
Huber, George W.
Huber, George W.
中科院分区:
化学2区
文献类型:
--
作者:
Jonathan, Alvin;Eagan, Nathaniel M.;Bruns, David L.;Stahl, Shannon S.;Lanci, Michael P.;Dumesic, James A.;Huber, George W.

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在这里,我们表明,C4-C12线性烯烃,包括线性α烯烃,可以选择性地由乙烯在稳定的钴氧化物碳催化剂上生产。当催化剂稳定时,本体和表面钴相都是CoO,这表明CoO是用于齐聚的稳定钴相。在反应期间,聚乙烯在催化剂孔中形成,这影响产物选择性。催化剂在较高温度(约200 °C)下更稳定,可能是由于Co 3 O 4还原成CoO,而在较低温度下观察到快速失活(例如,80-140 °C)。产物选择性可以拟合两种不同的Schulz Flory分布,一种是C4-C10烯烃,一种是C10以上烯烃,表明传输限制影响产物选择性。在48.3%的转化率下,C12烯烃的产物线性度高于90%,使其成为迄今为止在不存在活化剂和/或溶剂的情况下对线性烯烃最具选择性的非均相催化剂。
Here, we show that C4–C12 linear olefins, including linear alpha olefins, can be selectively produced from ethylene over a stable cobalt oxide on carbon catalyst. Both bulk and surface cobalt phases are CoO when the catalyst is stable, suggesting CoO is the stable cobalt phase for oligomerization. During the reaction, polyethylene forms in the catalyst pores which influences the product selectivity. The catalyst is more stable at higher temperatures (∼200 °C) likely due to reduction of Co3O4 to CoO while rapid deactivation is observed at lower temperatures (e.g., 80–140 °C). The product selectivity can be fit to two different Schulz Flory distributions, one from C4 to C10 olefins and one above C10 olefins, suggesting that transport restrictions influence product selectivity. At 48.3% conversion, product linearities up to C12 olefins are above 90%, making it the most selective heterogeneous catalyst to linear olefins to date in the absence of activators and/or solvents.
氧化钴碳催化剂上的烯烃二聚:I. 丙烯二聚
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