氧合物
合成气
沸石
选择性
化学
化学工程
催化作用
工程类
有机化学
作者
Chengtao Wang,Jian Zhang,Gangqiang Qin,Liang Wang,Erik Zuidema,Qi Yang,Shanshan Dang,Chengguang Yang,Jianping Xiao,Xiangju Meng,C.M.A.M. Mesters,Feng‐Shou Xiao
出处
期刊:Chem
[Elsevier]
日期:2020-03-01
卷期号:6 (3): 646-657
被引量:140
标识
DOI:10.1016/j.chempr.2019.12.007
摘要
The direct transformation of syngas into C2-oxygenates (e.g., ethanol) is in great demand, but it is still challenging because of the low selectivity and poor catalyst stability. Here, we overcome the issues and report a zeolite-fixation methodology to strengthen the transformation. By employing the extensively investigated RhMn catalyst, the silicate-1 zeolite-fixed RhMn nanoparticles with core-shell structure ([email protected]) exhibit high efficacy for the C2 oxygenates production from syngas, giving oxygenate selectivity at 40.3% under CO conversion of 42.4% (C2-oxygenate selectivity at 88.3% in the total oxygenates), which decidedly outperforms the previous catalysts in direct syngas-to-ethanol transformation. Multiple studies demonstrate that the rigid zeolite framework efficiently stabilizes the Mn-O-Rhδ+ structure, known as the crucial site for C2-oxygenate formation. In the long-term test, the [email protected] catalyst exhibits constant C2-oxygenate productivities with superior durability. This investigation demonstrates the powerful siliceous zeolite support in the C2-oxygenate production, which has not been explored previously.
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