Direct Conversion of Syngas to Ethanol within Zeolite Crystals

Direct Conversion of Syngas to Ethanol within Zeolite Crystals
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沸石晶体内合成气直接转化为乙醇

DOI:
10.1016/j.chempr.2019.12.007
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发表时间:
2020-03
期刊:
影响因子:
23.5
通讯作者:
Xiao Feng-Shou
Xiao Feng-Shou
中科院分区:
化学1区
文献类型:
--
作者:
Wang Chengtao;Zhang Jian;Qin Gangqiang;Wang Liang;Zuidema Erik;Yang Qi;Dang Shanshan;Yang Chengguang;Xiao Jianping;Meng Xiangju;Mesters Carl;Xiao Feng-Shou

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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 (RhMn@S-1) exhibit high efficacy for the C2oxygenates 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 RhMn@S-1 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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