Kang Jincan, He Shun, Zhou Wei, Shen Zheng, Li Yangyang, Chen Mingshu, Zhang Qinghong, Wang Ye
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Nat Commun. 2020 Feb 11;11(1):827. doi: 10.1038/s41467-020-14672-8.
Synthesis of ethanol from non-petroleum carbon resources via syngas (a mixture of H and CO) is an important but challenging research target. The current conversion of syngas to ethanol suffers from low selectivity or multiple processes with high energy consumption. Here, we report a high-selective conversion of syngas into ethanol by a triple tandem catalysis. An efficient trifunctional tandem system composed of potassium-modified ZnO-ZrO, modified zeolite mordenite and Pt-Sn/SiC working compatibly in syngas stream in one reactor can afford ethanol with a selectivity of 90%. We demonstrate that the K-ZnO-ZrO catalyses syngas conversion to methanol and the mordenite with eight-membered ring channels functions for methanol carbonylation to acetic acid, which is then hydrogenated to ethanol over the Pt-Sn/SiC catalyst. The present work offers an effective methodology leading to high selective conversion by decoupling a single-catalyst-based complicated and uncontrollable reaction into well-controlled multi-steps in tandem in one reactor.
通过合成气（H₂和CO的混合物）从非石油碳资源合成乙醇是一个重要但具有挑战性的研究目标。目前合成气转化为乙醇存在选择性低或多步过程能耗高的问题。在此，我们报道了通过三重串联催化将合成气高选择性转化为乙醇。一个由钾改性的ZnO-ZrO₂、改性丝光沸石和Pt-Sn/SiC组成的高效三功能串联体系，在一个反应器中于合成气流中协同工作，可实现乙醇选择性达90%。我们证明K-ZnO-ZrO₂催化合成气转化为甲醇，具有八元环孔道的丝光沸石用于甲醇羰基化生成乙酸，然后乙酸在Pt-Sn/SiC催化剂上氢化生成乙醇。本工作提供了一种有效的方法，通过将基于单催化剂的复杂且不可控的反应解耦为在一个反应器中串联的可控多步反应，实现高选择性转化。
