The design of new nanomaterials for rapid and reversible detection of molecules in existence is critical for real-world sensing applications. Current nanomaterial libraries such as carbon nanotubes, graphene, MoS2, and MXene are fundamentally limited by their slow detection speed and small signals; thus, the atomic-level material design of molecular transport pathways and active binding sites must be accompanied. Herein, we fully explore the chemical and physical properties of a hydrogen-substituted graphdiyne (HsGDY) for its molecular sensing properties. This new carbon framework comprises reactive sp carbons in acetylenic linkages throughout the 16.3 Å nanopores and allows for detecting target molecules (e.g., H2) with an exceptionally high sensitivity (ΔR/Rb = 542%) and fast response/recovery time (τ90 = 8 s and τ10 = 38 s) even without any postmodification process. It possesses 2 orders of magnitude higher sensing ability than that of existing nanomaterial libraries. We demonstrate that rapid and reversible molecular binding is attributed to the cooperative interaction with adjacent double sp carbon in the layered nanoporous structure of HsGDY. This new class of carbon framework provides fundamental solutions for nanomaterials in reliable sensor applications that accelerate real-world interfacing.
Keywords: channel material; chemiresistive sensor; graphdiyne; molecular sensing; nanoporous material.