I think that will be the climax of episode 4. She leaves in the beginning of the episode, but on her way, she's kidnapped by Smee. When Charming, Rumpel and Red finally rescue her, she's still angry at Rumpel and demands an explanation. And that's when he tells her about the curse and what happened to Baelfire.
I agree. Episode 4 is rumored to be a big episode for Rumpel. Jane Espenson tweeted that it’s her favorite episode so far, and so did Jennifer Morrison. Which is odd considering she’s not even in that episode. 😆