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More efficient ethanol synthesis from dimethyl ether and syngas over the combined nano-sized ZSM-35 zeolite with CuZnAl catalyst
Catalysis Today ( IF 5.3 ) Pub Date : 2020-03-19 , DOI: 10.1016/j.cattod.2020.03.035
Xiaobo Feng , Jie Yao , Yan Zeng , Yu Cui , Shun Kazumi , Reubroycharoen Prasert , Guangbo Liu , Jinhu Wu , Guohui Yang , Noritatsu Tsubaki

Converting syngas into ethanol (EtOH) is highly attractive but remains challenge. Dimethyl ether (DME) carbonylation with CO to methyl acetate (MA) on zeolite and its further hydrogenation to EtOH on Cu-based catalyst open a new EtOH synthesis route from syngas. In this work, a nano-sized ZSM-35 (NZ35) zeolite, possessing abundant active sites and porosity and short diffusion path, is found to realize much better activity of DME to MA than that of the conventional ZSM-35 zeolite (CZ35). In addition, a simple formic-acid-assisted solid-state method is employed for preparation an auto-reduced CuZnAl (CZAargon) catalyst under argon atmosphere. The prepared CZAargon catalyst exhibits an excellent catalytic activity for conversion of produced MA to EtOH. By investigating the effects of different integration manners of NZ35 zeolite and CZAargon catalyst, we find that EtOH can be synthesized only when the NZ35 zeolite and CZAargon catalyst pack in a dual-catalyst bed reactor. After optimizing the reaction conditions for EtOH synthesis with the combination of NZ35 zeolite and CZAargon catalyst, it is found that the DME conversion and MA selectivity are stabilized at 47.0 % and 45.6 % respectively, at 220 °C and 2.5 MPa.



中文翻译:

纳米ZSM-35沸石与CuZnAl催化剂在二甲醚和合成气上更有效地合成乙醇

将合成气转化为乙醇(EtOH)极具吸引力,但仍面临挑战。在沸石上用CO将二甲醚(DME)羰基化为乙酸甲酯(MA),然后在基于铜的催化剂上将其进一步加氢为EtOH,这开辟了一条新的合成气EtOH合成路线。在这项工作中,发现具有丰富活性位点和孔隙率且扩散路径短的纳米级ZSM-35(NZ35)沸石比常规ZSM-35沸石(CZ35)具有更好的DME对MA的活性。 。此外,采用简单的甲酸辅助固态法在氩气气氛下制备自动还原的CuZnAl(CZA)催化剂。准备好的CZA氩气催化剂对于将生成的MA转化为EtOH表现出极好的催化活性。通过研究NZ35沸石和CZA催化剂不同整合方式的影响,我们发现只有当NZ35沸石和CZA催化剂在双催化剂床反应器中堆积时,才能合成EtOH 。在使用NZ35沸石和CZA氩气催化剂优化EtOH合成的反应条件后,发现DME的转化率和MA的选择性分别在220°C和2.5 MPa时稳定在47.0%和45.6%。

更新日期:2020-03-19
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