4.7 Article

In situ construction of an immobilized b-oriented titanium silicalite spherical molecular sieve membrane

Journal

APPLIED SURFACE SCIENCE
Volume 563, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apsusc.2021.150275

Keywords

TS-1; Molecular sieve membrane; B-orientation; In situ crystallization; Immobilized catalyst

Funding

  1. National Natural Science Youth Fund Project of China [21706289]
  2. Fundamental Research Funds for the Central Universities [20CX02211A]
  3. State Key Laboratory of Heavy Oil Processing

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In this study, a single layer of b-oriented continuous titanium silicalite-1 (TS-1) molecular sieve membrane was successfully prepared on the surface of 2-mm alumina beads, providing a foundation for the design of novel TS-1 immobilized catalyst. The directional growth of molecular sieve membranes on spherical substrates has not been reported before, and the membrane showed potential in catalyzing the epoxidation of chloropropene with high conversion and selectivity.
Oriented molecular sieve membranes prepared on the surface of a specifically shaped substrate have been applied in the separation and catalysis process, but there is no report on the directional growth of molecular sieve membranes on the surface of spherical substrates. Here, a simple in situ crystallization method was employed to successfully prepare a single layer of b-oriented continuous titanium silicalite-1 (TS-1) molecular sieve membrane on the surface of 2-mm alumina beads. First, a titania intermediate layer was loaded on the surface of beads by the dipping method, and the surface was then modified with the TBOT modification solution. The ratio of the precursor solution was n(TEOS):n(TBOT):n(TPAOH):n(H2O) = 1:0.010:0.15:40 and was crystallized at 180 degrees C for 72 h to prepare the membrane. The content of the templating agent and water affected the size of TS-1 crystal grains and membrane crosslinking-both in turn influenced the continuity and orientation of the molecular sieve membrane. Spherical membrane catalyst was applied to catalyze the epoxidation of chloropropene in a fixed bed reactor, and the conversion of hydrogen peroxide and selectivity of epichlorohydrin attained 87.4% and 93.2%, respectively. This work provides a foundation for the design of novel TS-1 immobilized catalyst.

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