The computer probably won't let your program use ALL of the memory on the system, so you are stuck. There is no way to "force" the computer to give you memory when it doesn't have any (or doesn't want) to give.
You man need to directly to the OS with VirtualAlloc. But before you do, think about what you mean by maximum free memory. This is not a fixed measure in a multi-processor/multi-user/virtual memory system, and it may not mean what you think it means.