it's a worthy experiment. There's a good chance that the Valkyrie video controller won't address more than 1MB of VRAM, or that the address lines are not present, but who knows. The Hardware developer note (
http://mirror.informatimago.com/next/developer.apple.com/documentation/Hardware/Developer_Notes/Macintosh_CPUs-68K_Desktop/Mac_LC_630_Quadra_630.pdf) pg. 16, says that the Valkyrie is similar to the display portion of the MEMCjr in the Q605 (1MB limit) and the DAFB in the Q700 and Q900 (2 MB?). The note also says that the video memory is plain old RAM, not any special dual ported RAM or such.
Late edit: and the note says there's 8MB of address space allocated to VRAM. Doesn't mean much, but at least it's not limited to 1MB. Figure 2-2, pg. 19.
One megabyte of memory, thirty-two bits wide, in 8 chips is made of 8 1Mbit chips which are each 4 bits wide. So, 256K X 4 chips, X 8. If you want to double that, then you need to find 512K X 4 chips. The pinout will be standard. 256K means that there are 18 address bits, and at least 9 address pins on each chip (addresses are multiplexed, sent 1/2 at a time). If there are only 9 address pins, then it can't be done, absent discovering an unused DRAM address pin on the Valkyrie chip. 512K X n memory chips require at least 10 address pins.
However, there is a tiny bit of hope, as the 256K chips could be addressed in an 8 X 10 or 10 X 8 pattern instead of 9 X 9, in which case 10 address pins would be present.
As someone else wrote, the first step should be to identify the VRAM chips and find a datasheet for them.
Oh, one last thing, memory capacities of chips seemed to always increase by factors of 4, so 512K X 4 chips may not exist. You may have to go to 1M X 4. That can still work with 10 address pins though, so if there are 10 the first hurdle is cleared.
It looks like I have a bunch of Oki MSM514400D 1M X 4 chips on hand, somewhere in the attic. These are also what the super common 4MB 32 pin SIMM would have usually have built out of, so you can salvage them from those too.
Looking at the datasheet for the M2M514400, the chip has 20 pins in a 26 pin pattern. I.e. There are two rows of pins with room for 13 pins, but the middle 3 pins in each row are omitted.
View attachment MSM514400E.pdf