Abstract
This work shows unprecedented data on stabilizing H+-MFI during 1-butene oligomerization into C12-C16 products. The stable catalytic behavior, with mean lives beyond 103 h, is attributed to an extended olefin liquid-phase within MFI capillaries containing H+ species. The narrow pores in MFI and the isolated H+ sites allow rigorous assessments of void walls in catalysis. The primary character of the oligomerization products minimize secondary readsorption chances and oligomerization events from products. Such mechanistic pathway seems independent of the phase, but narrow MFI pores that enable intrapore liquids lead to a remarkable stabilization of 1-C4 conversion and product selectivity. This is confirmed by analyzing used MFI solids via thermogravimetry, indicative of the solvating role of capillary liquids. This work remarkably extends this knowledge into H+-catalysts (Brönsted acid-sites) that lead to strongly bound alkoxides. The studied zeolites and high 1-C4 conversion represent a promising landmark to translate new concepts into industrial requirements.
Published Version
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