Replacing is always the better option. Adding memory to existing memory results in mixed memory and there are never any guarantees that will work or that they'll play nice together.
Anytime you plan to use more than one module, for dual, triple or quad channel operation, is is ALWAYS a good idea to buy them in a matched, tested set that is already known to work together. Even buying IDENTICAL part numbers is no guarantee that any two modules will work together because there are so many variables involved. Usually there is some room for compatibility differences, but a LOT of the time, more and more as time goes on and systems become more specifically finicky to differences in hardware, there is not.
Modules with the part number XXXX...