Graphene oxide-based large-area dynamic covalent interfaces

Dynamic materials, being capable of reversible structural adaptation in response to the variation of external surroundings, have experienced significant advancements in the past several decades. In particular, dynamic covalent materials (DCMs), where the dynamic covalent bonds (DCBs) can reversibly break and reform under defined conditions, present superior dynamic characteristics, such as self-adaptivity, self-healing and shape memory. However, the dynamic characteristics of DCBs are mainly limited within the length scale of covalent bonds, due to the local position exchange or the inter-distance variation between the chemical compositions involved in the reversible covalent reactions. In this minireview, a discussion regarding the realization of long-range migration of chemical compositions along the interfaces of graphene oxide (GO)-based materials via the spatially connected and consecutive occurrence of DCB-based reversible covalent reactions is presented, and the interfaces are termed "large-area dynamic covalent interfaces (LDCIs)". The effective strategies, including water adsorption, interfacial curvature and metal-substrate support, as well as the potential applications of LDCIs in water dissociation and humidity sensing are summarized. Additionally, we also give an outlook on potential strategies to realize LDCIs on other 2D carbon-based materials, including the interfacial morphology and periodic element doping. This minireview provides insights into the realization of LDCIs on a wider range of 2D materials, and offers a theoretical perspective for advancing materials with long-range dynamic characteristics and improved performance, including controlled drug delivery/release and high-efficiency (bio)sensing.