4.6 Article

Microfibrous-Structured SS-fiber@meso-HZSM-5 Catalyst for Methanol-to-Propylene: Steam-Assisted Crystallization Synthesis and Insight into the Stability Enhancement

Journal

ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 5, Issue 2, Pages 1840-1853

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.6b02567

Keywords

Structured catalyst; ZSM-S; Steam-assisted crystallization; Mesopore; Methanol-to-propylene

Funding

  1. NSF of China [21473057, 21322307, U1462129, 21273075]
  2. 973 program from the MOST of China [2011CB201403]

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Free-standing stainless-steel (SS)-fiber@meso-HZSM-5 core-shell catalysts engineered from micro-to macro-scale were highly efficiently synthesized via cost-effective steam-assisted crystallization (SAC) method. Impact of synthesis conditions on their morphology and textural/acidic properties was investigated by means of XRD, SEM, TEM, solid-state NMR, NH3-TPD, Py-IR and N-2 physisorption. 80 Single-run lifetime of such structured catalysts for MTP process was strongly dependent on their preparation conditions but slightly the product distribution. A volcano-like relationship for lifetime was observed against the SAC time, which was correlated well with the crystallization-time-dependent crystallinity, mesoporosity and crystal size. The promising SS-fiber@meso-HZSM-5 was the one obtained after the SAC for 12 h, which delivered a prolonged single-run lifetime of 620 h with a high propylene selectivity of similar to 42% at 450 degrees C using a methanol weight hourly space velocity (WHSV) of 1 h(-1), as the result of high crystallinity, well-developed mesoporosity and small crystal size. Note that well-developed mesoporosity was paramount for the catalyst stability improvement, because of enhanced accommodation capacity of zeolite shell for receiving formed coke.

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