You posted this in the "After 1900" so no.
However if Portugal had merged into Spain since long, yes, I believe that the geopolitical psyche of a unified peninsula would soften separatist tendencies in Catalonia. With that said, a united Great Britain doesn't eliminate Scottish separatism. Whatever drives one nation to perceive itself as a nation and to go as far as to want independence is much more than geographic perception albeit I don't devalue the concept at all.