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Get 64gb 4x16 first and if it would work well to your expectations, then add another kit.
I have tested 64GB 3600 and it works no errors with MemTest. When adding the additional 2-4 sticks (+96GB/128GB), it starts throwing crazy errors. At 3600 it is unstable and the system will freeze within 10 minutes (tested under Windows).
At 3466 there was no system freeze for the whole kit, but a bunch of errors in Memtest and tiny issues like laggy cursor sometimes etc. But no system freezes.
I'm currently back on Crucial Ballistix Sport LT 64GB kit (4x16GB, 2400M/T) and no issues here and have returned the GSKILL kit for now until I figure stuff out.
Also it's important to get a whole kit since their serial numbers are consecutive...at least when you have so many DIMMs.