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A Grimoire is a book of magic, as Beelzebub explains in Lesson 6-4. Several of them exist, and they represent a demon's soul, as stated in Lesson 14-10. Grimoires are very powerful magical objects; they have the power to control a demon and make them do anything, even if it's in violation of a pact. Barbatos also mentions in Lesson 53-4 that by reading a demon's Grimoire, one could learn everything there is to know about said demon.
Main Story and Events
In Lesson 53, Solomon reveals that he possesses Barbatos's grimoire, which Barbatos says he trusted Solomon with of his own free will. In Lessons 54, whether Barbatos actually gave Solomon his grimoire or not is put into question when he admits the grimoire given to MC was a fake.