The main 3 unlimited decks I have already utterly destroy the opponent on the first turn that you're allowed to play trainers, without needing unlimited copies of a card.
One of the three would benefit immensely from extra Scoop Ups though.
Deck 1. Use Crobat's Flash Bite as many times as possible to spread approximately 30-40 damage counters on the first turn. Could definitely use more Scoop Ups.
Deck 2. Using Fossil Vileplume, Fossil Aerodactyl, and Aggron ex, prevent your opponent from evolving, attacking, or using powers or bodies or trainers. The only existing card that would break the lock is Cyclone Energy, so you just make sure you get a second Aggron ex on the bench.
Deck 3. Using Blastoise ex, Espeon, and Forretress, place unlimited damage on your opponent's Pokemon who's names are not Forretress. Pokemon Center or Alakazam/Quagsire are both fine ways of removing damage from your side as you go.
Now that I think of it, all three would actually benefit immensely from being allowed to play any number of Erika, as Erika is without compare the best draw card in existence, especially if you could play more than 4. I'm pretty sure all three of these decks run 4/4/4/4/4 Bill/Erika/Prof Oak/CPU Search/Item Finder except maybe the first one because you need to cram as many Scoop Up-like cards in as possible (Scoop Up, PokeTurn, Mr. Fuji, and then 50%'ers like SSU)