"wrath; meaning extreme anger"
so for this I'd say Pan, followed by Regina or Rumple.

Definitely Hook since his anger and wrath has controlled most of his life after his brother died and has gotten worse when Rumple both sliced off his hand but more importantly killed his beloved right in front of him.

To be honest all of them are bad with this one. Villains tend to have extreme anger. Maybe not Cora, she didn't seem as angry as the others.

Or Rumps.

She had enough wrath to create the curse. But most of them are big with this one.

To be honest I feel like Cora and Pan are the only ones that don't suit this one. Pan and Cora are just too calculated. They don't ever let there emotions take control.

Def!

All of them.

Taking everything into consideration I would say Regina suits this sin the most.

Wrath (Latin, ira), also known as "rage", may be described as inordinate and uncontrolled feelings of hatred and anger. Wrath, in its purest form, presents with self-destructiveness, violence, and hate that may provoke feuds that can go on for centuries. Wrath may persist long after the person who did another a grievous wrong is dead. Feelings of anger can manifest in different ways, including impatience, revenge, and self-destructive behavior

Rumple, Regina and Zelena are all tied in my books.

Also Killian/Hook. Regina edged it in this because of her scapegoating the wrong target for her revenge, and the extremes she went to get that revenge.