Metal Ion‐induced Gelation of High‐concentration Graphite‐like Crystalline Nanosheet Aqueous Suspensions

Abstract The stability and transformation of nanomaterial aqueous suspensions are essential for their applications. Preparation of high‐concentration carbon nanomaterials suspensions remains challenging due to their nonpolar nature. Herein, 200 mg mL⁻¹ carbon nanomaterial aqueous suspensions are achieved by using graphite‐like crystalline nanosheets (GCNs) with high hydrophilicity. Furthermore, these high‐concentration GCN aqueous suspensions spontaneously transform into gels when induced by mono‐, di‐, and trivalent metal salt electrolytes at room temperature. Theoretical calculation of potential energy by DLVO theory reveals that the gelatinized GCNs is a new and metastable state between two usual forms of solution and coagulation. It is shown that the gelation of GCNs is due to the preferential orientation of nanosheets in an edge‐edge arrangement, which differs from the case of solution and coagulation. High‐temperature treatment of GCN gels produces metal/carbon materials with pore structures. This work provides a promising opportunity to create various metal/carbon functional materials.