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在ZnCrO + H-SSZ-13双功能催化剂上合成气直接转化为轻质烯烃

Direct Conversion of Syngas to Light Olefins over a ZnCrO + H-SSZ-13 Bifunctional Catalyst.

作者信息

Huang Yuxuan, Ma Hongfang, Xu Zhiqiang, Qian Weixin, Zhang Haitao, Ying Weiyong

机构信息

Engineering Research Center of Large Scale Reactor Engineering and Technology, Ministry of Education, State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China.

出版信息

ACS Omega. 2021 Apr 19;6(16):10953-10962. doi: 10.1021/acsomega.1c00751. eCollection 2021 Apr 27.

Abstract

In recent years, bifunctional catalysts for the syngas-to-olefins (STO) reaction via the oxide-zeolite (OX-ZEO) strategy has been intensively investigated. However, the bifunctional catalyst containing H-SSZ-13 with a 100% H-exchanging degree for the STO reaction has not been developed because of the high selectivity to paraffin. Here, we report a ZnCrO + H-SSZ-13 bifunctional catalyst, which contains the submicron H-SSZ-13 with adequate acidic strength. Light olefins in hydrocarbon reached 70.8% at a CO conversion of 20.9% over the ZnCrO + H-SSZ-13(23S) bifunctional catalyst at 653 K, 1.0 MPa, and GHSV = 6000 mL·g·h after 800 min of STO reaction. The effect of CO and H on the C-C coupling was discussed by carrying out the methanol-to-olefins (MTO) reaction under a similar atmosphere as that of the STO reaction. H and CO should play a more dominant role than the conventional hydrogen transfer reaction on the undesired high selectivity of paraffins. These findings provide new insight into the design of the bifunctional catalyst for the STO process via the OX-ZEO strategy.

摘要

近年来,通过氧化物-沸石(OX-ZEO)策略用于合成气制烯烃(STO)反应的双功能催化剂受到了广泛研究。然而,由于对石蜡的高选择性,尚未开发出用于STO反应的具有100%氢交换度的含H-SSZ-13双功能催化剂。在此,我们报道了一种ZnCrO + H-SSZ-13双功能催化剂,其包含具有适当酸性强度的亚微米级H-SSZ-13。在653 K、1.0 MPa和GHSV = 6000 mL·g·h的条件下,经过800分钟的STO反应,在ZnCrO + H-SSZ-13(23S)双功能催化剂上,当CO转化率为20.9%时,烃类中的轻质烯烃达到了70.8%。通过在与STO反应类似的气氛下进行甲醇制烯烃(MTO)反应,讨论了CO和H对C-C偶联的影响。H和CO在石蜡不希望有的高选择性上,应比传统的氢转移反应发挥更主要的作用。这些发现为通过OX-ZEO策略设计用于STO过程的双功能催化剂提供了新的见解。

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