▎ 摘　　要

There have been growing academic interests in the study of strong organic molecule-graphene [or graphene oxide (GO)] systems, owing to their essential noncovalent nature and the consequent chemomechanical behavior within the interface. A more recent experimental measurement [Chem 2018, 4, 896-910] reported that the melamine-GO interface exhibits a remarkable noncovalent binding strength up to similar to 1 nN, even comparable with typical covalent bonds. But the poor understanding on the complex noncovalent nature in particular makes it challenging to unveil the mystery of this high-performance interface. Herein, we carry out first-principles calculations to investigate the atomistic origin of ultrastrong noncovalent interaction between the melamine molecule and the GO sheet, as well as the chemomechanical synergy in interfacial behavior. The anomalous O-H center dot center dot center dot N hydrogen bonding, formed between the triazine moiety of melamine and the -OH in GO, is found cooperatively enhanced by the pin-like NH2-pi interaction, which is responsible for the strong interface. Following static pulling simulations validates the 1 nN level rupture strength and the contribution of each noncovalent interaction within the interface. Moreover, our results show that the -OH hydrogen bonding will mainly augment the interfacial adhesion strength, whereas the -NH2 group cooperating with the -OH hydrogen bonding and conjugating with the GO surface will greatly improve the interfacial shear performance. Our work deepens the understanding on the chemomechanical behaviors within the noncovalent interface, which is expected to provide new potential strategies in designing high-performance graphene-based artificial nacreous materials.