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Regulating anisotropic diffusion in zeolite for reinforced para-xylene synthesis via CO2 hydrogenation in the presence of toluene.

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Title: Regulating anisotropic diffusion in zeolite for reinforced para-xylene synthesis via CO2 hydrogenation in the presence of toluene.
Authors: Shang, Xin1,2 (AUTHOR), Han, Jingfeng1 (AUTHOR), Han, Qiao1 (AUTHOR), Hou, Guangjin1 (AUTHOR), Zheng, Anmin3,4 (AUTHOR), Yang, Xiaofeng1 (AUTHOR), Liu, Zhiqiang1,3,4 (AUTHOR) zqliu_wh@wust.edu.cn, Liu, Guodong1 (AUTHOR) gdliu@dicp.ac.cn, Su, Xiong1 (AUTHOR) suxiong@dicp.ac.cn, Huang, Yanqiang1 (AUTHOR), Zhang, Tao1,2 (AUTHOR)
Source: Applied Catalysis B: Environment & Energy. Dec2024, Vol. 359, pN.PAG-N.PAG. 1p.
Subjects: Carbon dioxide, Xylene, Zeolites, Hydrogenation, Isomers
Abstract: The synthesis of valuable aromatics via CO 2 transformation, especially para -xylene (PX), is of paramount significance but still remains greatly challenging due to the low efficiency and poor selectivity. The present work utilized a composite catalyst based on ZnZrO x with a modified H-ZSM-5 exhibiting nano-prism stacking to realize the selective synthesis of PX. Methoxy species generated from CO 2 -derived formate produced as an intermediate over the ZnZrO x were readily incorporated into the xylene products for effective alkylation, contributed to an enhanced aromatics-based cycle that provided a selectivity for xylenes among all C 5+ hydrocarbons of 91.1 %. The lengthened straight channels in the H-ZSM-5 along the b -axis, derived from the crystal stacking pattern, increased differences in the diffusion properties of the xylene isomers, and thereby steering the movement of molecules toward a product shape-selective pathway, leading to 90.1 % selectivity for PX among all xylenes, and provided exceptional CO 2 utilization efficiency of ∼60 %. [Display omitted] • 90 % xylene containing 90 % PX was produced in aromatics over ZnZrO x &C-Z5. • Tandem reaction mechanism contributes the high yield of xylene. • Stacking structure oriented along specific axis regulates the anisotropic product diffusion. • Lengthened diffusion path in straight channel reinforce selective synthesis of PX. [ABSTRACT FROM AUTHOR]
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Database: Engineering Source
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Abstract:The synthesis of valuable aromatics via CO 2 transformation, especially para -xylene (PX), is of paramount significance but still remains greatly challenging due to the low efficiency and poor selectivity. The present work utilized a composite catalyst based on ZnZrO x with a modified H-ZSM-5 exhibiting nano-prism stacking to realize the selective synthesis of PX. Methoxy species generated from CO 2 -derived formate produced as an intermediate over the ZnZrO x were readily incorporated into the xylene products for effective alkylation, contributed to an enhanced aromatics-based cycle that provided a selectivity for xylenes among all C 5+ hydrocarbons of 91.1 %. The lengthened straight channels in the H-ZSM-5 along the b -axis, derived from the crystal stacking pattern, increased differences in the diffusion properties of the xylene isomers, and thereby steering the movement of molecules toward a product shape-selective pathway, leading to 90.1 % selectivity for PX among all xylenes, and provided exceptional CO 2 utilization efficiency of ∼60 %. [Display omitted] • 90 % xylene containing 90 % PX was produced in aromatics over ZnZrO x &C-Z5. • Tandem reaction mechanism contributes the high yield of xylene. • Stacking structure oriented along specific axis regulates the anisotropic product diffusion. • Lengthened diffusion path in straight channel reinforce selective synthesis of PX. [ABSTRACT FROM AUTHOR]
ISSN:09263373
DOI:10.1016/j.apcatb.2024.124523