Nanoscale corrugations induced by structural evolution in graphene oxide nanosheets and their unexpected catalytic...

Nanoscale corrugations, a distinct conformational feature of monolayer two-dimensional materials, possess unique atomic bonding characteristics and electrical properties. However, their inherent instability and the lack of effective engineering strategies have posed significant challenges to investigating their catalytic activities in conventional chemical reactions. Here, we present a facile and scalable method to induce nanoscale corrugations in graphene oxide (GO) nanosheets through controlled structural evolution. By harnessing the intrinsic chemical and structural metastability of GO, suspended nanosheets spontaneously collapsed into well-aligned corrugated patterns via phase separation during alkali-acid annealing. These self-triggered nanotextures display notable mechanical robustness and retain their morphology throughout the reaction process. The resulting corrugated GO (CGO) exhibits remarkably enhanced catalytic activity, achieving superior nitrobenzene conversion and improved aniline selectivity. The observed reaction rate constant (k_obs) is approximately twice that of pristine planar GO (PGO), which is attributed to the preferential adsorption and local accumulation of nitrobenzene and H₂S molecules along the corrugated sidewalls. This work not only demonstrates the feasibility of regulating nanoscale conformations in suspended GO via structural evolution but also reveals the overlooked catalytic potential of corrugations. It further highlights the unexpected chemical and physical properties that may arise in corrugated regions of other 2D materials.