Note that to safely re-assign the device to the pool you need to do this:
Stop the array, if Docker/VM services are using the cache pool disable them, unassign the remaining cache device, start array to make Unraid "forget" current cache config, stop array, now reassign both cache devices (there can't be an "All existing data on this device will be OVERWRITTEN when array is Started" warning for any cache device), re-enable Docker/VMs if needed, start array, then do the remove procedure.