The sorption and reaction of but-1-ene over a ferrierite sample was studied by in situ IR spectroscopy to relate the selectivity to isobutene and the sorbed species. The spectra highlighted the presence of various unsaturated species including polyenes, which were readily formed upon contacting H-FER with but-1-ene while a poor selectivity to isobutene was observed. Aromatic compounds were concluded to be subsequently formed via dehydrogenation/cyclization of the polyenic deposits while the isobutene selectivity increased via suppression of by-products. These data support earlier assumptions that the initial high yield of by-products was produced by the reaction of butenes with reactive deposits, which were gradually converted into more inert aromatic deposits. Upon purging the catalyst with an inert, branched C8 hydrocarbons and aromatic molecules such as xylenes desorbed. The rates of desorption showed an initially linear variation with the square root of time and were fitted to a monodimensional Fickian model. Because the slowly diffusing species were rather abundant during the course of the reaction, it is proposed that the skeletal isomerization was effectively limited to the acid sites close the pore mouth of H-FER crystallites.