They actually address some of that on their project page, see: https://llvm-mos.org/wiki/Findings
I suspect that an LLVM backend for the 816 would have to be something quite a bit different from the 02.
I personally would choose the 65x816 over the other for a new design, but I can understand why it’s not as popular.
[0]: 40 was the de facto maximum. Although, the M68k had 64. That thing was a monster in size.