Influence of zinc state on the catalyst properties of Zn/HZSM-5 zeolite in 1-hexene aromatization and cyclohexane dehydrogenation

doi:10.1016/j.cjche.2022.01.005

中国化学工程学报 ›› 2022, Vol. 43 ›› Issue (3): 124-134.DOI: 10.1016/j.cjche.2022.01.005

Influence of zinc state on the catalyst properties of Zn/HZSM-5 zeolite in 1-hexene aromatization and cyclohexane dehydrogenation

Di Gao¹, Yibo Zhi¹, Liyuan Cao¹, Liang Zhao¹, Jinsen Gao¹, Chunming Xu¹, Mingzhi Ma², Pengfei Hao²

1. State Key Laboratory of Heavy Oil Processing, China University of Petroleum (Beijing), Beijing 102249, China;
2. Hebei Jingzhi Technology Company Limited, Cangzhou 061000, China

收稿日期:2021-09-10 修回日期:2021-12-24 出版日期:2022-03-28 发布日期:2022-04-28
通讯作者: Liang Zhao,E-mail:liangzhao@cup.edu.cn
基金资助:
The authors acknowledge the support from the National Natural Science Foundation of China (21838011).

Influence of zinc state on the catalyst properties of Zn/HZSM-5 zeolite in 1-hexene aromatization and cyclohexane dehydrogenation

Di Gao¹, Yibo Zhi¹, Liyuan Cao¹, Liang Zhao¹, Jinsen Gao¹, Chunming Xu¹, Mingzhi Ma², Pengfei Hao²

1. State Key Laboratory of Heavy Oil Processing, China University of Petroleum (Beijing), Beijing 102249, China;
2. Hebei Jingzhi Technology Company Limited, Cangzhou 061000, China

Received:2021-09-10 Revised:2021-12-24 Online:2022-03-28 Published:2022-04-28
Contact: Liang Zhao,E-mail:liangzhao@cup.edu.cn
Supported by:
The authors acknowledge the support from the National Natural Science Foundation of China (21838011).

摘要/Abstract

摘要： Rational design of Zn-containing HZSM-5 zeolite (Zn/HZSM-5) with high reactivity and excellent aromatization performance for olefin aromatization is crucially desired. We develop a new and uncomplicated method to synthesize Zn/HZSM-5 (IMX/Z5) with superior aromatization performance in the paper. Compared to incipient wetness impregnation (IMP/Z5) and mechanical mixing (MIX/Z5), the as-prepared IMX/Z5 presents a higher amount of surface ZnOH⁺ species (2.87%) while keeping identical bulk zinc content. As a result, more surface ZnOH⁺ favor both the aromatization of 1-hexene and cyclohexane dehydrogenation. For the two olefin aromatization pathways (hydrogen transfer and dehydrogenation), it is the first time found both the hydrogen transfer ability and the dehydrogenation ability increase linearly with the amount of surface ZnOH⁺ species while keeping identical bulk zinc content. We believe that the linear relationships are essential to design next generation olefin aromatization catalysts.

关键词: Zinc state, Catalyst, Catalysis, Hydrogen transfer, Dehydrogenation, Moleclar sieves

Abstract: Rational design of Zn-containing HZSM-5 zeolite (Zn/HZSM-5) with high reactivity and excellent aromatization performance for olefin aromatization is crucially desired. We develop a new and uncomplicated method to synthesize Zn/HZSM-5 (IMX/Z5) with superior aromatization performance in the paper. Compared to incipient wetness impregnation (IMP/Z5) and mechanical mixing (MIX/Z5), the as-prepared IMX/Z5 presents a higher amount of surface ZnOH⁺ species (2.87%) while keeping identical bulk zinc content. As a result, more surface ZnOH⁺ favor both the aromatization of 1-hexene and cyclohexane dehydrogenation. For the two olefin aromatization pathways (hydrogen transfer and dehydrogenation), it is the first time found both the hydrogen transfer ability and the dehydrogenation ability increase linearly with the amount of surface ZnOH⁺ species while keeping identical bulk zinc content. We believe that the linear relationships are essential to design next generation olefin aromatization catalysts.

Key words: Zinc state, Catalyst, Catalysis, Hydrogen transfer, Dehydrogenation, Moleclar sieves

Di Gao, Yibo Zhi, Liyuan Cao, Liang Zhao, Jinsen Gao, Chunming Xu, Mingzhi Ma, Pengfei Hao. Influence of zinc state on the catalyst properties of Zn/HZSM-5 zeolite in 1-hexene aromatization and cyclohexane dehydrogenation[J]. 中国化学工程学报, 2022, 43(3): 124-134.

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Influence of zinc state on the catalyst properties of Zn/HZSM-5 zeolite in 1-hexene aromatization and cyclohexane dehydrogenation

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