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The relations of crystallite sizes over Silicalite-1 zeolite with the silanols distribution and catalytic performance in methanol to propene (MTP) reaction were determined. The catalytic lifetime and the formation of ethene was independent of the crystallite size, but was attributed to the silanols distribution. The internal isolated silanol groups (I) affects the diffusion restrictions of intermediate species. The external isolated silanols (E) determined the tolerance for coke capacity on the external surface. Propene and the initial catalytic activity was dominated by the amount of Brønsted acid sites.