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A 64 or even a 128 should work, but can you actually use the extra memory?
For each doubling of size, 16/32/64/128 you need another physical address line to access the extra memory. This has to be a circuit on the motherboard and also the software must accommodate it.
If you have a spare 64G kicking around with nowhere to use it, it should work the same as a 32G. Hardly worth buying one special though as the prices will likely go down before you can actually use the full capacity in an ereader.
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