4.6 Article

Methanol to olefins: activity and stability of nanosized SAPO-34 molecular sieves and control of selectivity by silicon distribution

Journal

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 15, Issue 35, Pages 14670-14680

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cp52247d

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Funding

  1. Spanish MINECO [MAT2012-37160, CSD2009-00050-CONSOLIDER/INGENIO 2010]
  2. Generalitat Valenciana by the PROMETEO program
  3. China Scholarship Council (CSC)
  4. State Basic Research Project of China [2011CB808703]
  5. National Natural Science Foundation of China

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Nano-SAPO-34 molecular sieves synthesized in a microwave environment with 20 nm crystal size showed a longer lifetime than SAPO-34 prepared by the conventional hydrothermal method in the reaction of methanol to olefins. It has been found that silicon distribution strongly affects the lifetime and selectivity. Thus, silicon at the border of the silicon islands gives a higher lifetime and lower C2/C3 ratio. This change in activity and selectivity is better explained in terms of different silicon distribution than by preferential diffusion of ethene through the 8MR pores and agrees with transition-state selectivity. The effects of equilibrium of olefins and deactivation by coke were isolated, showing that after full formation of the hydrocarbon pool, selectivity is independent of deactivation by coke.

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