Assuming VCR/0042 is correct then you want to look at Rob's list of advanced codes for VCR/0042 at
[Link: hifi-remote.com]There are other threads here (such as that "unofficial manual" thread) that tell you how to use KeyMover to bind any of those three digit EFC numbers to keys.
If I'm understanding your request right, you need some functions that are on the original remote that aren't bound to keys by VCR/0042. If the correct EFC numbers for those functions are in that list then I've already answered your question. If the EFC numbers are wrong or missing or I misunderstood the question, ask again with a little more specifics.