That wouldn't add fault tolerance. In fact, it would increase the likelihood of failure - because you'd be putting more stress on the physical drive.
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It won't work with RAID because you need drives of the same general size, but you could make a mirror of the NVME onto the other drives I suppose. I don't see any benefit to this though. It kinda sounds like you're creating a solution to a problem that doesn't exist here. You also probably won't see any performance benefit to using the 500GB as a read cache for a number of reasons, so maybe consider if you absolutely and desperately REALLY wanna use those two slots, just buy two drives and make a volume out them. Simplifies your setup quite a bit.
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