U+221F, U+2227鈥揢+222A and U+228C鈥揢+228E are placed on the baseline rather than being centered on the math axis. They also seem to be a bit small. The U+2229 and U+222A should probably be more similar in appearance to a rotated U+2282.
The + and 脳 are only included in the image for reference.

It is always good idea to check what other math fonts are doing here and what happens when the math font is used by a math layout engine (*TeX math mode, for example).
It's the same in XeTeX and Word. All other maths fonts I have are correctly aligned, so are other symbols in Libertinus.
Note to self or anybody else that works on this: while checking math symbol alignment also review whether +lnum vs. +onum features do/should affect what center line is used. See example this comment on Elstob.
Clearly @thlinard is somebody to ping to review alignment when a PR is ready for this :wink:!
Hey @philosaurus, see #454 for dicussion about resolving this issue. I am also pinging @thlinard concerning the alignment discussion in the same place.