Harnessing Holey MXene/Graphene Oxide Heterostructure to Maximize Ion Channels in Lamellar Film for High‐Performance Capacitive Deionization

Abstract 2D Ti 3 C 2 T x MXene‐based film electrodes with metallic conductivity and high pseudo‐capacitance are of considerable interest in cutting‐edge research of capacitive deionization (CDI). Further advancement in practical use is however impeded by their intrinsic limitations, e.g., tortuous ion diffusion pathway of layered stacking, vulnerable chemical stability, and swelling‐prone nature of hydrophilic MXene nanosheet in aqueous environment. Herein, a nanoporous 2D/2D heterostructure strategy is established to leverage both merits of holey MXene (HMX) and holey graphene oxide (HGO) nanosheets, which optimize ion transport shortcuts, alleviate common restacking issues, and improve film's mechanical and chemical stability. In this design, the nanosized in‐plane holes in both handpicked building blocks build up ion diffusion shortcuts in the composite laminates to accelerate the transport and storage of ions. As a direct outcome, the HMX/rHGO films exhibit remarkable desalination capacity of 57.91 mg g −1 and long‐term stability in 500 mg L −1 NaCl solution at 1.2 V. Moreover, molecular dynamics simulations and ex situ wide angle X‐ray scattering jointly demonstrate that the conductive 2D/2D networks and ultra‐short ion diffusion channels play critical roles in the ion intercalation/deintercalation process of HMX/rHGO films. The study paves an alternative design concept of freestanding CDI electrodes with superior ion transport efficiency.