4.8 Article

Selective Introduction of Acid Sites in Different Confined Positions in ZSM-5 and Its Catalytic Implications

Journal

ACS CATALYSIS
Volume 8, Issue 8, Pages 7688-7697

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b02112

Keywords

zeolites; DFT; Al siting; boron ZSM-5; MTO; catalytic cracking

Funding

  1. European Union [ERC-AdG-2014-671093]
  2. Spanish Government-MINECO through Severo Ochoa [SEV-2016-0683]
  3. China Scholarship Council (CSC)
  4. [CTQ2015-70126-R]

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Controlling the location of acid sites in zeolites can have a great effect on catalysis. In this work we face the objective of directing the location of AI into the 10R channels of ZSM-5 by taking advantage of the structural preference of B to occupy certain positions at the channel intersections, as suggested by theoretical calculations. The synthesis of B-Al-ZSM-5 zeolites with variable Si/Al and Si/B ratios, followed by B removal in a postsynthesis treatment, produces ZSM-5 samples enriched in Al occupying positions at 10R channels. The location of the acid sites is determined on the basis of the product distribution of 1-hexene cracking as a test reaction. The higher selectivity to propene and lower C-4(=)/C-3(=) ratio in the samples synthesized with B and subsequently deboronated can be related to a larger concentration of acid sites in 10R channels, where monomolecular cracking occurs. Finally, several ZSM-5 samples have been tested in the methanol to propene reaction, and those synthesized through the B -assisted method show longer catalytic lifetime, higher propene yield, and lower yield of alkanes and aromatics.

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