I would like a double two-finger touchbar tap to invoke the "pause/play" methods. But, I do not see any sorts of doubletaps in touchbar gestures.
Also, the play/pause thing seems to just focus on whatever media it thinks is playing. If I have podcasts playing, but then a video is on reddit or something, play/pause no longer pauses the podcast. I don't think this is BBT's fault though. But, I miss the old days when F7 or something always paused iTunes, no matter what was playing.