High CO conversion in syngas to aromatics by addition of ZnMnZr oxides as methanol synthesis components†

IF 3.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Shiyu Liu, Qiuyun Huang, Jie Wang, Weihua Shen and Yunjin Fang
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Abstract

In the oxide-zeolite (OX-ZEO) strategy, it is challenging to achieve both higher CO conversion and aromatics selectivity. In this paper, the methanol synthesis component xZn2Mn8Zr was prepared. With increasing Zn content, CO conversion over the ternary oxides increased without a remarkable decrease in the combined selectivity of methanol and dimethyl ester (DME). The 2Zn2Mn8Zr (molar ratio) was then coupled with either SAPO-34 or H-ZSM-5 for syngas conversion. Combined with the results of thermogravimetric analysis, a bifunctional catalyst with more residual hydrocarbon pool species (HCPs) was capable of achieving higher selectivity of unsaturated organic products. The loss of HCPs should be attributed to over-hydrogenation. The over-hydrogenation could be related to either Zn concentration or the close contact of 2Zn2Mn8Zr with H-ZSM-5. To alleviate such over-hydrogenation, ZnMnZr pellets with lower Zn concentration were mixed with the pellets of 6Mn4Zr/H-ZSM-5 using a granule mixing method. The multi-functional catalyst exhibited much higher activity in syngas-to-aromatics (STA) conversion, especially at high space velocities. The CO conversion over the multi-functional catalyst could reach 43% at 600 mL gcat−1 h−1, with aromatics selectivity around 72%, and it remained stable during a 100 h reaction.

Abstract Image

添加ZnMnZr氧化物作为甲醇合成组分,可提高合成气中CO的芳烃转化率
在氧化物-沸石(OX-ZEO)策略中,既要实现较高的CO转化率,又要实现芳烃选择性是一个挑战。本文制备了甲醇合成组分xZn2Mn8Zr。随着Zn含量的增加,CO在三元氧化物上的转化率增加,但甲醇和二甲酯(DME)的联合选择性不显著降低。然后将2Zn2Mn8Zr(摩尔比)与SAPO-34或H-ZSM-5偶联进行合成气转化。结合热重分析结果表明,含有较多残余烃池物质(HCPs)的双功能催化剂对不饱和有机产物具有较高的选择性。HCPs的损失应归因于过度氢化。过氢化反应可能与Zn浓度有关,也可能与2Zn2Mn8Zr与H-ZSM-5的密切接触有关。为了缓解这种过氢化现象,采用混粒法将Zn浓度较低的ZnMnZr球团与6Mn4Zr/H-ZSM-5球团混合。该多功能催化剂在合成气制芳烃(STA)转化中表现出较高的活性,特别是在高空速下。在600 mL gcat−1 h−1条件下,该催化剂的CO转化率可达43%,芳烃选择性约为72%,在100 h的反应时间内保持稳定。
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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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