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In my small vocal booth (3x6, 7.5' high), is it better to use one of the 3" panels on the ceiling? (instead of putting a 1.5" / 3pcf panel on the ceiling, and using all the 6pcf on the walls/corners).
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Yes if you can go with the 3". BTW 3pcf will work very well.
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is 1/4" a sufficient amount of space between the panel frame and the wall?
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If that is all you the space leave then go for it.
The rule of thumb though is to put equal air space, the thickness of the panel. So if the panel is 3" of mineral wool then leave a 3" air gap.
Glenn