Issue 20, 2018

Design of efficient bifunctional catalysts for direct conversion of syngas into lower olefins via methanol/dimethyl ether intermediates

Abstract

The direct conversion of syngas into lower olefins is a highly attractive route for the synthesis of lower olefins. The selectivity of lower olefins via the conventional Fischer–Tropsch (FT) synthesis is restricted to ∼60% with high CH4 selectivity due to the limitation by the Anderson–Schulz–Flory (ASF) distribution. Here, we report the design of bifunctional catalysts for the direct conversion of syngas into lower olefins with selectivity significantly breaking the ASF distribution. The selectivity of C2–C4 olefins reached 87% at a CO conversion of 10% and was sustained at 77% by increasing CO conversion to 29% over a bifunctional catalyst composed of Zn-doped ZrO2 nanoparticles and zeolite SSZ-13 nanocrystals. The selectivity of CH4 was lower than 3% at the same time. It is demonstrated that the molar ratio of Zn/Zr, the density of Brønsted acid sites of SSZ-13 and the proximity of the two components play crucial roles in determining CO conversion and lower-olefin selectivity. Our kinetic studies indicate that methanol and dimethyl ether (DME) are key reaction intermediates, and the conversion of syngas to methanol/DME is the rate-determining step over the bifunctional catalyst. Formate and methoxide species have been observed on Zn-doped ZrO2 surfaces during the activation of CO in H2, and the formed methanol/DME are transformed into lower olefins in SSZ-13.

Graphical abstract: Design of efficient bifunctional catalysts for direct conversion of syngas into lower olefins via methanol/dimethyl ether intermediates

Supplementary files

Article information

Article type
Edge Article
Submitted
08 apr. 2018
Accepted
29 apr. 2018
First published
30 apr. 2018
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2018,9, 4708-4718

Design of efficient bifunctional catalysts for direct conversion of syngas into lower olefins via methanol/dimethyl ether intermediates

X. Liu, W. Zhou, Y. Yang, K. Cheng, J. Kang, L. Zhang, G. Zhang, X. Min, Q. Zhang and Y. Wang, Chem. Sci., 2018, 9, 4708 DOI: 10.1039/C8SC01597J

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. You can use material from this article in other publications, without requesting further permission from the RSC, provided that the correct acknowledgement is given and it is not used for commercial purposes.

To request permission to reproduce material from this article in a commercial publication, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party commercial publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements