The impact of the zeolite Bronsted and Lewis acid site concentration on the catalytic cracking of alkanes was explored using n-pentane and H-ZSM-5 as examples. Rates normalized to strong Bronsted acid sites (i.e., the turnover frequencies, TOF) showed that the two samples with the highest Al content had much higher TOF than all other samples. This difference has been unequivocally linked to the presence of extra-lattice alumina. Post-treatment of the zeolites with ammonium hexafluorosilicate and static calcination was used to vary the concentration of extra-lattice alumina. After extraction of extra-lattice alumina from the samples with high TOF, all TOFs were identical. IR spectra of adsorbed pyridine and NH3, coupled with (27)AI MAS NMR, showed that the overall enhanced activity is associated with tetrahedrally coordinated extra-lattice alumina in close proximity to strong Bronsted acid sites. The TOF of these sites is approximately 40-times higher than the TOF on normal Bronsted acid sites. (C) 2014 Elsevier Inc. All rights reserved.