Rational Design of Zinc/Zeolite Catalyst: Selective Formation of p-Xylene from Methanol to Aromatics Reaction

Ning Wang; Jing Li; Wenjing Sun; Yilin Hou; Lan Zhang; Xiaomin Hu; Yifeng Yang; Xiao Chen; Congmei Chen; Biaohua Chen; Weizhong Qian

doi:10.1002/anie.202114786

Rational Design of Zinc/Zeolite Catalyst: Selective Formation of p-Xylene from Methanol to Aromatics Reaction

Angew Chem Int Ed Engl. 2022 Mar 1;61(10):e202114786. doi: 10.1002/anie.202114786. Epub 2022 Feb 4.

Authors

Ning Wang¹, Jing Li², Wenjing Sun³, Yilin Hou⁴, Lan Zhang¹, Xiaomin Hu¹, Yifeng Yang⁴, Xiao Chen⁴, Congmei Chen⁵, Biaohua Chen¹, Weizhong Qian⁴

Affiliations

¹ Faculty of Environment and Life, Beijing University of Technology, Beijing, 100124, China.
² Department of Chemistry, Tsinghua University, Beijing, 100084, China.
³ China-America Cancer Research Institute, Key Laboratory for Medical Molecular Diagnostics of Guangdong Province, Guangdong Medical University, Dongguan, Guangdong, 523808, China.
⁴ Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
⁵ National Supercomputing Center in Shenzhen, Shenzhen Cloud Computing Center), Guangdong, Shenzhen, 518055, China.

PMID: 35037354
DOI: 10.1002/anie.202114786

Abstract

The production of p-xylene from the methanol to aromatics (MTA) reaction is challenging. The catalytic stability, which is inversely proportional to the particle size of the zeolite, is not always compatible with p-xylene selectivity, which is inversely proportional to the external acid sites. In this study, based on a nano-sized zeolite, we designed hollow triple-shelled Zn/MFI single crystals using the ultra-dilute liquid-phase growth technique. The obtained composites possessed one ZSM-5 layer (≈30 nm) in the middle and two silicalite-1 layers (≈20 nm) epitaxially grown on two sides of ZSM-5, which exhibited a considerably long lifetime (100 % methanol conversion >40 h) as well as an enhanced shape selectivity of p-xylene (>35 %) with a p-xylene/xylene ratio of ≈90 %. Importantly, using this sandwich-like zeolite structure, we directly imaged the Zn species in the micropores of only the ZSM-5 layer and further determined the specific structure and anchor location of the Zn species.

Keywords: Hollow Zeolite; Methanol Conversion; Triple Shell; Zinc; p-Xylene.

Abstract

Grants and funding