A Kindle is a really crappy candidate for this, especially a KT4.
You’re correct in mentioning that the SoC would support the capabilities that you’re after but it’s not a given that the relevant pins are broken on as a test point on the PCB in the first place or that they’re not already used by one of the built in peripherals.
I’m not sure that it’s even possible to edit/reflash the DTB on the later devices (PW4, KT4 onwards) without hard bricking the device due to the whole secure boot thing?
For this use case I’d seriously consider using a Kobo instead - contrast having to figure out a novel, low level method of adding storage vs just popping out the SD card and cloning it to a larger one.
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