The Simpler the Better: Ultrafast Air‐Plasma Synthesis of 3D Crosslinked Graphene Nanoscroll‐Nanosheet Aerogels at Room Temperature for Capacitive Deionization

Abstract Graphene nanoscroll (GNS) is an important 1D tubular form of graphene‐derivative materials, which has garnered widely attention. However, conventional fabrication methods commonly suffer from complex processing and time‐consuming. Herein, with graphene oxide (GO) as a precursor, the study puts forward a facile air‐plasma synthesis strategy to fabricate 3D graphene nanoscroll‐nanosheet aerogels (GSSA). It is demonstrated that without using any chemical additives, a highly efficient reduction‐exfoliation‐scrolling process can be achieved all‐in‐one at room temperature within 1 s. The GNSs “grew” from 2D graphene sheets and firmly cross‐linked them together, and they not only provide a shortcut path for electron transport but also act as intrinsic spacers to prevent restacking of graphene sheets. When using as an electrode material for capacitive deionization (CDI), GSSA exhibits excellent merits of salt‐removal performance. These findings open a new pathway to large‐scale synthesis of high‐quality and high‐purity GNS‐based materials with promising applications in CDI and beyond.