He’s jealous.
Hades and Persephone now have a powerful cultus in Eleusis, and they are rising stars in the pantheon.
And from his perspective, Hades nearly destroyed the world over a girl… over his insistence on keeping her even though Demeter was starving the earth. He, in a way, expected more from him, and expected Aidon to be the rational well reasoned one.
Zeus’s big motivation in life is to keep the peace between around 30 or so dieties who are all powerful enough to wipe humanity off the face of the earth. And while this couple, who are amassing more and more worshipers, they also represent an ideal of marriage that Zeus cannot live up to.
They both threaten to upend the ordered, patriarchal system he has had in place for aeons, they have made seasonal change a constant, which will have bigger ramifications later, and he can’t really forgive them for that.