Air-gap-assisted solvothermal process to synthesize unprecedented graphene-like two-dimensional TiO2 nanosheets for Na+ electrosorption/desalination

Designing a high-performance capacitive deionization setup is limited due to the slow salt removal and charge storage capacities. Efforts are being made to replace traditional electrodes with advanced 2D materials. We introduce a simple method for synthesizing two-dimensional titanium dioxide graphene-like nanosheets via a unique air-gap-assisted solvothermal method. Crystalline 2D graphene-like anatase-TiO2 sheets of unprecedented quality were obtained by tuning the air gap in the solvothermal reactor. The 2D TiO2 synthesized by air-gap-assisted solvothermal process has shown an exceptionally high surface area of 934.5 m2/g compared to the pristine TiO2 (249.5 m2/g). The sheets were used as Faradaic electrodes in ion-electrosorption and their capacitive deionization capabilities were evaluated. The electrochemical conductivity was examined via an in situ investigation of Na+-ion migration and storage. The adsorption capacity of 2D TiO2 sheets increased with higher applied potential while keeping the adsorption time constant at 15 min. At adsorption potentials of –0.8 V, –1.0 V, and –1.2 V, desalting rates of 2.09, 2.18, and 2.20 mg g−1 min−1 resulted in adsorption capacities of 31.33, 32.73, and 33.023 mg g–1, respectively. The 2D TiO2 electrode demonstrated high electron-transfer rates, a large desalination capacity, and a rapid average desalting rate. The specific capacity of the 2D-layered TiO2 electrode was found to be about 45.68 F g−1. These results can be attributed to the large specific surface area, short ionic diffusion paths, numerous active adsorption sites, surface defects, and pseudocapacitance. This air-gap-assisted solvothermal method is expected to open new avenues for the synthesis of high-quality 2D materials.