Which does "his mouth full of brimstone" most likely mean?

This phrase is typically used figuratively to describe someone who is speaking harshly, critically, or in a way that is heavily flavored with threats or condemnation. It may also suggest a person who is angry, bitter, or intense in their speech. In religious contexts, "brimstone" is often associated with the fires of hell or damnation, so the phrase can also carry a connotation of wrath or divine punishment.