If an 8GB module is less than twice the price of a 4GB module, it is more economical to buy the 8GB instead, and leaves slots open for future expansion.
Do not buy 16GB modules, and they are ALL "Registered" DIMMs and will not mix freely and play nice with non-registered DIMMs, Regardless, when the new DIMMs arrive, test the new ones by themselves FIRST, then add the old ones back and test again. This separates "does not work" problems from "will not play nice with others" problems.
always buy from a Vendor who says:
"It works in your Mac
or your money Back!"
I would add datamemorysystems to that list:
http://www.datamemorysystems.com/apple-mac-pro-quad-core-intel-xeon-nehalem-2-66 ghz-mb871ll/a-early-2009-memory-upgrades…
.