Journal
CHEM
Volume 6, Issue 3, Pages 646-657Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2019.12.007
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Funding
- National Key Research and Development Program of China [2018YFB0604801]
- National Natural Science Foundation of China [21822203, 91645105, 91634201, 91945302, 91845103]
- Natural Science Foundation of Zhejiang Province [LR18B030002]
- Fundamental Research Funds for the Central Universities [2019XZZX004-02]
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The direct transformation of syngas into C-2-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 C-2 oxygenates production from syngas, giving oxygenate selectivity at 40.3% under CO conversion of 42.4% (C-2-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-Rh delta+ structure, known as the crucial site for C-2-oxygenate formation. In the long-term test, the RhMn@S-1 catalyst exhibits constant C-2-oxygenate productivities with superior durability. This investigation demonstrates the powerful siliceous zeolite support in the C-2-oxygenate production, which has not been explored previously.
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