MBR's sector addresses are 32-bits. This means there can only be 2^32 (=~ 4 billion) addressable sectors. With the hardware using 512 byte sectors, this yields both a maximum disk and partition size of 2^32 * 512 == 2 terabytes.
In theory with a drive that uses >612B sectors would support larger disk sizes under MBR, but crucially SD cards, even the latest SDUC, still use 512 byte blocks.
As already mentioned, In order to utilize more than 2TB on a single physical drive (note the quad iflash adapter counts as a "single" drive in this context), Rockbox would need support for GPT partitions (not that difficult) but critically also would need to move to 64-bit addressing throughout the storage stack. But even once that's in place, FAT32 is still limited to 32-bit sector counts, yielding the same 2TB partition size limit on 512-byte sector drives.
ExFAT blows away those limits, but would be a significant undertaking to implement.