4.6 Article

Influence of Tetrapropylammonium and Ethylenediamine Structure-Directing Agents on the Framework Al Distribution in B-Al-MFI Zeolites

Journal

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
Volume 58, Issue 27, Pages 11849-11860

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.9b01726

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Funding

  1. National Science Foundation, an Engineering Research Center for the Innovative and Strategic Transformation of Alkane Resources (CISTAR) [EEC-1647722]

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We report synthetic protocols to independently influence composition and crystallite sizes of MFI zeolites, properties that contribute to Thiele moduli, and the proximity of Al heteroatoms at fixed composition (Si/Al similar to 50). Crystallite sizes decrease with the addition of non-catalytic B heteroatoms in B-Al-MFI zeolites. Using only tetra-n-propylammonium (TPA(+)) as a structure-directing agent (SDA) leads to occlusion of one TPA(+) per channel intersection and a finite percentage of framework Al atoms (20-40%) in proximal configurations. In contrast, using mixtures of ethylenediamine (EDA) and TPA(+) (EDA/TPA(+) = 15) leads to incorporation of EDA that displaces some TPA(+) and to nearly all (>95%) Al in isolated configurations. These findings indicate how adding B and EDA to zeolite synthesis solutions provides a route to crystallizing MFI zeolites of similar composition but with framework Al distributed at varying relative proximity, or with similar Al distributions but different diffusion path lengths.

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