4.8 Article

Construction of a One-Dimensional Al-Rich ZSM-48 Zeolite with a Hollow Structure

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 46, Pages 52025-52034

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c16346

Keywords

ZSM-48 zeolite; diffusion limitation; acidity; hollow structure; m-xylene isomerization

Funding

  1. National Natural Science Foundation of China [22172162, U20A20120]
  2. BP Energy Innovation Laboratory [EIL-045]
  3. Dalian Innovation Team in Key Areas [2020RT06]
  4. STS Network Initiative [KFJ-STS-QYZD-2021-17-001/002]
  5. Strategic Priority Research Program of the CAS [XDA 21000000]

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A hollow Al-rich ZSM-48 zeolite with improved diffusion ability and acid density has been successfully synthesized through an alumination-recrystallization strategy, solving the challenges of diffusion limitation and acid deficiency. The obtained zeolite shows excellent catalytic stability and high p-xylene yield, indicating its strong potential for industrial applications.
Diffusion limitation and acid deficiency are two main challenges that the ZSM-48 zeolite faces in practical application. To date, there have been few effective strategies to solve both problems, simultaneously. Also, it is also a challenge to construct a hollow structure in a one-dimensional (1D) zeolite. Herein, an Al-rich ZSM-48 zeolite with a hollow structure is constructed through an alumination-recrystallization strategy, thereby solving the problems related to diffusion and acidity simultaneously. The hollowness and enrichment of aluminum can be controlled by judiciously matching the desilication and recrystallization. The silica to alumina ratio (SAR) of the ZSM-48 zeolite can be tuned from 130 to 45, which breaks the SAR limitation of conventional synthesis. On the basis of the different characterization results, the whole crystallization can be divided into two stages: rapid desilication-alumination and time-consuming recrystallization. In the selective desilication-recrystallization process, the preferential special distribution of the organic template leads to the formation of a hollow structure and the healing of mesopores at the outer shell, as evidenced by structured illumination microscopy images. Due to the enhancement in diffusion ability and acid density, the obtained hollow Al-rich ZSM-48 zeolite exhibits excellent catalytic stability and high p-xylene yield (& SIM;26%) in the m-xylene isomerization reaction (WHSV = 18 h-1), indicating its strong industrial application potential.

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