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Direct Conversion of Syngas to Ethanol within Zeolite Crystals
Chem ( IF 23.5 ) Pub Date : 2020-01-16 , DOI: 10.1016/j.chempr.2019.12.007
Chengtao Wang , Jian Zhang , Gangqiang Qin , Liang Wang , Erik Zuidema , Qi Yang , Shanshan Dang , Chengguang Yang , Jianping Xiao , Xiangju Meng , Carl Mesters , Feng-Shou Xiao

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.



中文翻译:

沸石晶体中合成气直接转化为乙醇

合成气直接转化为C 2-含氧化合物(例如乙醇)的需求量很大,但由于选择性低和催化剂稳定性差,仍然具有挑战性。在这里,我们克服了这些问题,并报告了一种固定沸石的方法来加强转化。通过使用经过广泛研究的RhMn催化剂,具有核-壳结构([电子邮件保护])的硅酸盐-1沸石固定的RhMn纳米颗粒对合成气产生的C 2含氧化合物具有很高的效力,在CO转化为CO的情况下,含氧化合物的选择性为40.3%。 42.4%(C 2-含氧化合物在总含氧化合物中的选择性为88.3%),在直接合成气向乙醇的直接转化中,其性能明显优于先前的催化剂。多项研究表明,刚性沸石骨架有效地稳定了Mn-O- Rhδ +结构,该结构被称为C 2含氧化合物形成的关键部位。在长期测试中,[受电子邮件保护的]催化剂具有恒定的C 2-含氧化合物生产率,并具有出色的耐久性。这项研究证明了在C 2-含氧化合物生产中强大的硅质沸石载体,这是以前没有探索过的。

更新日期:2020-01-16
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