The effects of cations on the local electromagnetic environments of catalytic sites in Y-zeolites are studied as a function of cation type and concentration. Quadrupolar coupling parameters measurable using Al-27 MAS NMR at multiple field strengths, provide a window to study aluminum's local electronic structure. Quadrupolar parameters calculated for framework tetrahedral aluminum are related to cation concentration and Bronsted acidity for potassium-, zinc-, and lanthanum-exchanged NH4NaY and USY zeolites.