Do you mean atoms at the vertices or also endohedral trapped atoms within?
Anyway it seems theoretically there should be no limit- if you increase the radius you can make any number of C atoms at vertices. But whether in practices such higher fullerenes remain stable or self sustained above say C=84 or somewhat larger is the question. The cage will no longer remain spherical or semi-spherical but will flatten like a normal 3-D stuff if you increase the number. What critical number will sustain a cage like structure depends upon apart from atom-atom interactions, but also masses of atoms involved.