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通过多功能催化剂上的合成气转化直接生产高含氧化合物

Direct Production of Higher Oxygenates by Syngas Conversion over a Multifunctional Catalyst.

作者信息

Lin Tiejun, Qi Xingzhen, Wang Xinxing, Xia Lin, Wang Caiqi, Yu Fei, Wang Hui, Li Shenggang, Zhong Liangshu, Sun Yuhan

机构信息

CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201203, China.

University of Chinese Academy of Sciences, Beijing, 100049, China.

出版信息

Angew Chem Int Ed Engl. 2019 Mar 26;58(14):4627-4631. doi: 10.1002/anie.201814611. Epub 2019 Feb 28.

Abstract

Selective synthesis of higher oxygenates (linear α-alcohols and α-aldehydes, C OH) from syngas is highly attractive but remains challenging owing to the low C OH selectivity and low catalytic stability. Herein we introduce a multifunctional catalyst composed of CoMn and CuZnAlZr oxides that dramatically increased the oxygenates selectivity to 58.1 wt %, where more than 92.0 wt % of the produced oxygenates are C OH. Notably, the total selectivity to value-added chemicals including oxygenates and olefins reached 80.6 wt % at CO conversion of 29.0 % with high stability. The appropriate component proximity can effectively suppress the formation of the undesired C1 products, and the selectively propulsion of reaction network by synergetic effect of different components contributes to the enhanced selectivity to higher oxygenates. This work provides an alternative strategy for the rational design of new catalysts for direct conversion of syngas into higher oxygenates with co-production of olefins.

摘要

由合成气选择性合成高级含氧化合物(线性α-醇和α-醛,CₓOH)极具吸引力,但由于CₓOH选择性低和催化稳定性差,仍然具有挑战性。在此,我们介绍一种由CoMn和CuZnAlZr氧化物组成的多功能催化剂,该催化剂可将含氧化合物的选择性显著提高至58.1 wt%,其中超过92.0 wt%的生成含氧化合物为CₓOH。值得注意的是,在CO转化率为29.0%时,包括含氧化合物和烯烃在内的增值化学品的总选择性达到80.6 wt%,且具有高稳定性。适当的组分邻近性可以有效抑制不需要的C1产物的形成,不同组分的协同作用对反应网络的选择性推进有助于提高对高级含氧化合物的选择性。这项工作为合理设计用于将合成气直接转化为高级含氧化合物并联产烯烃的新型催化剂提供了一种替代策略。

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