Interesting. This sort of thing is highly bios specific, I'm running 240G of VRAM on a single box using a very simple config:

GRUB_CMDLINE_LINUX_DEFAULT="pcie_aspm=off amd_iommu=on iommu=pt pci=realloc,firmware noapic nomodeset pci=nommconf gpu_unlock.targets=0000:66:00.0,0000:69:00.0,0000:6d:00.0,0000:6e:00.0"

The gpu_unlock is a bit hacky (but I have many GPUs that the unlock won't work on and that will cause issues), and there are two BIOS settings that matter: above 4GB decode enabled and resizeable bar enabled. That's it.