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As long as you have an EU ID you should be good

If on a visa you may well have to reapply. Visas are given out on a country by country basis.

Take a lol here

Thank you everyone for your responses. We will make a trip to Spain this summer and ask many questions while there. Thanks again!

We would like to travel from Madrid to Barcelona by train. Is there a recommended website where I can purchase the tickets in advance of our trip? Thank you!

If you are US expats, your residency and visas for Portugal would NOT be any good in Spain. Each nation has its own process for non-EU nationals. Having residency permission in one EU nation does not entitle you to move to another EU nation.

The good news is that you would not need to go back to the US to apply. You can apply for a Spanish non-lucrative visa (retiree visa) in Portugal. You can always apply for that visa in a nation that you are legally residing in (so you would have to show the Spanish consulate in Portugal your Portuguese residency papers).