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I am trying to farm both Ectoplasm and Frozen Key Mold in Terraria.

If I place more than 300 blocks of ice/snow in the dungeon so that the background turn into ice, will killing dungeon mobs give me the Frozen Key Mold?

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If the wording on the Biome Key Mold wiki page is accurate, I believe the answer to your question is yes. From said page (emphasis is mine):

After the Wall of Flesh is defeated, every enemy has a 0.04% (1 in 2500) chance of dropping a Biome Key Mold. The type of Biome Key Mold that is dropped depends on the biome you are currently in (Jungle, Corruption, Crimson, Hallow or Snow). Any mold can drop in Ocean biomes.

Creating an artificial snow biome should eventually yield a frozen key mold, assuming that your character remains within that biome. You'd need to make the biome big enough to ensure that you don't accidentally exit it and enter back into the natural dungeon.

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The best way to farm the frozen key mold is to build enough Meteorite blocks in the ice biome, so that the little Meteorites spawn. Add a Water Candle to increase the spawning rates. Get the items that have AFK damage (end-game armors sometimes have a guardian or turret ability) and let it go to work.

For the dungeon, my best way to get ectoplasm was just to keep running through and kill everything. Stay in areas with water candles or place them yourself.

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    As of 1.2.3 Meteor heads no longer drop loot in hardmode, including key molds. – VanBuzzKill Feb 15 '15 at 2:45
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    This doesn't really answer the question in the OP, either. – John Cleaver Feb 15 '15 at 17:01

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