1. Are we pretty sure all the best enslave mobs have been found? I can think of a few that, on paper, seem like they'd be pretty good but that I've never seen in use. Maybe not enslavable?
Biggest limit is going to be the level of the mob. For example, your not going to enslave those nice orcs by the siege camp, because their level is too close to 50. Your not going to slave high level giant mobs for the same reason. There are some mobs (exiled orc shaman for example) that are just not slavable for some reason or another even though they are the right race.
3. Can you enslave a mob in combat? If not, could you spinebreak it, then enslave it while combat is stopped?
If your thinking about enslaving agro mobs, I would guess anything that was aggor and enslavable would be cowed by bully anyway. If you fail enslave you have to spinebreak before you can try again
I can't remember enslaving a troll. Ogres, hobgoblins, goblins orcs. I've never had any luck getting to the edge though so (I blame RNG on skill improves)