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Success! I now have 128GB of flash storage and a gargantuan battery - something like four and a half times the original battery capacity.

I reformatted the SD card before starting. I've heard that modern exFAT cards sometimes come preformatted with a partition layout that confuses the iPod, so I did a full reformat and then recreated it as HFS+ since I'm going to be using it on a Mac.

Getting the iPod open's a bit of a chore, but I'm getting good at it now. The plastic iFlash tools help.