4.8 Article

High Stability of Methanol to Aromatic Conversion over Bimetallic Ca,Ga-Modified ZSM-5

Journal

ACS CATALYSIS
Volume 12, Issue 5, Pages 3189-3200

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c05481

Keywords

methanol-to-aromatics; bimetallic catalyst; dehydrogenation; global optimization; catalyst deactivation

Funding

  1. Advanced Research Center Chemical Building Blocks Consortium (ARC CBBC) [2016.007.TUD]
  2. European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme [725686]
  3. NWO Domain Science

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The addition of minute amounts of Ca can stabilize the catalyst and extend its lifetime. The interaction between Ca and Ga-LAS has an effect on the aromatization process.
The production of valuable aromatics and the rapid catalyst deactivation due to coking are intimately related in the zeolite-catalyzed aromatization reactions. Here, we demonstrate that these two processes can be decoupled by promoting the Ga/HZSM-5 aromatization catalyst with Ca. The resulting bimetallic catalysts combine high selectivity to light aromatics with extended catalyst lifetime in the methanol-to-aromatics process. Evaluation of the catalytic performance combined with detailed catalyst characterization suggests that the added Ca interacts with the Ga-LAS, with a strong effect on the aromatization processes. A genetic algorithm approach complemented by ab initio thermodynamic analysis is used to elucidate the possible structures of bimetallic extraframework species formed under reaction conditions. The promotion effect of minute amounts of Ca is attributed to the stabilization of the intrazeolite extraframework gallium oxide clusters with moderated dehydrogenation activity.

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