Journal
INORGANIC CHEMISTRY FRONTIERS
Volume 9, Issue 13, Pages 3348-3358Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2qi00686c
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Funding
- National Natural Science Foundation of China [22008019, 22002012, 21972013]
- China Postdoctoral Science Foundation [2021T140083]
- Open Sharing Fund for the Large-Scale Instruments and Equipment of Dalian University of Technology [DUTKFJJ2021128]
- Liao Ning Revitalization Talents Program [XLYC2008032]
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Applying consecutive SiO2-P2O5-MgO (SPM) and SiO2 surface coatings on ZSM-5 catalysts can achieve high para-selectivity, while loading Pt, Ni, and (Pt+Ni) metals can enhance catalytic stability. The study confirms that the most effective location for metal loading is on the external surface of the modified catalysts.
This work aims to achieve high para-selectivity while maintaining catalytic stability for the alkylation of toluene with methanol to para-xylene over ZSM-5 catalysts under demanding reaction conditions. A high para-selectivity of greater than 97% is achieved by applying consecutive SiO2-P2O5-MgO (SPM) and SiO2 surface coatings on the surface of pristine ZSM-5. This surface modification passivates the external acid sites and at the same time narrows the pore openings of the ZSM-5 particles, which are both beneficial for the high para-selectivity. The catalytic stability of the surface modified catalysts is achieved by loading with metals including Pt, Ni and (Pt + Ni). This study shows that catalysts co-loaded with (Pt + Ni) exhibit superior catalytic stability, not only in pure H-2 but also in a carrier gas containing a very low H-2 fraction of 5% H-2 and 95% Ar. This is because the co-existence of Pt and Ni effectively inhibits the formation of low-carbon olefins (the coke precursors) via the dehydrogenation of methanol to carbon oxides and the hydrogenation of olefins to paraffins. By studying the different locations of metal loading on the catalysts, this work also confirms that the most effective location of metal loading is on the external surface of the modified catalysts.
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