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Lee aluminum for me. Just can't justify the significant difference in expense for iron/steel moulds. The performance/price advantage just isn't there, aluminum is too inexpensive and works too well. That said I have a couple brass moulds obtained with cap and ball revolvers, and one iron/steel Lyman mold for round balls for my 12 gauge as Lee does not make the aluminum ones that large, and they all work fine.
As far as PC goes, pottery clay was a popular material for moulds, as was soapstone and other easily carved stone. Even animal tusks/horns were used:
"In the Field Museum of Natural History in Chicago there is an Inuit bullet mould that was hand-carved out of a single, split Walrus tusk. I stood staring at that display for quite some time, imagining the many long, cold, lonely nights spent carefully splitting, facing, hinging, and shaping that ivory in some remote igloo until the round balls that fell from it were just right for whatever musket that hardy soul used to feed himself with."
http://www.lasc.us/Fryxell_Book_Chapter_9_MouldsMouldDesign.htm
And while walrus tusk may be PC, it probably is not "PC" in today's world.
As far as PC goes, pottery clay was a popular material for moulds, as was soapstone and other easily carved stone. Even animal tusks/horns were used:
"In the Field Museum of Natural History in Chicago there is an Inuit bullet mould that was hand-carved out of a single, split Walrus tusk. I stood staring at that display for quite some time, imagining the many long, cold, lonely nights spent carefully splitting, facing, hinging, and shaping that ivory in some remote igloo until the round balls that fell from it were just right for whatever musket that hardy soul used to feed himself with."
http://www.lasc.us/Fryxell_Book_Chapter_9_MouldsMouldDesign.htm
And while walrus tusk may be PC, it probably is not "PC" in today's world.