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

2D Ti3C2Tx 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.

Hierarchically Porous 3D Freestanding Holey-MXene Framework via Mild Oxidation of Self-Assembled MXene Hydrogel for Ultrafast Pseudocapacitive Energy Storage.

The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode's charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (Ti3C2Tx) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH3)4]2+) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create nanoholes on the MXene surface. These hierarchically porous, conductive holey-MXene frameworks facilitate 3D transport of both electrons and electrolyte ions to deliver an excellent specific capacitance of 359.2 F g-1 at 10 mV s-1 and superb capacitance retention of 79% at 5000 mV s-1, representing a 42.2% and 15.3% improvement over pristine MXene hydrogel, respectively. Even at a commercial-standard mass loading of 10.1 mg cm-2, it maintains an impressive capacitance retention of 52% at 1000 mV s-1. This rational design of an electrode by engineering nanoholes on MXene nanosheets within a 3D porous framework dictates a significant step forward toward the practical use of MXene and other 2D materials in electrochemical energy storage systems.

Vacancy-Rich MXene-Immobilized Ni Single Atoms as a High-Performance Electrocatalyst for the Hydrazine Oxidation Reaction.

Single-atom catalysts (SACs), on account of their outstanding catalytic potential, are currently emerging as high-performance materials in the field of heterogeneous catalysis. Constructing a strong interaction between the single atom and its supporting matrix plays a pivotal role. Herein, Ti3 C2 Tx -MXene-supported Ni SACs are reported by using a self-reduction strategy via the assistance of rich Ti vacancies on the Ti3 C2 Tx MXene surface, which act as the trap and anchor sites for individual Ni atoms. The constructed Ni SACs supported by the Ti3 C2 Tx MXene (Ni SACs/Ti3 C2 Tx ) show an ultralow onset potential of -0.03 V (vs reversible hydrogen electrode (RHE)) and an exceptional operational stability toward the hydrazine oxidation reaction (HzOR). Density functional theory calculations suggest a strong coupling of the Ni single atoms and their surrounding C atoms, which optimizes the electronic density of states, increasing the adsorption energy and decreasing the reaction activation energy, thus boosting the electrochemical activity. The results presented here will encourage a wider pursuit of 2D-materials-supported SACs designed by a vacancy-trapping strategy.

A transport channel-regulated MXene membrane via organic phosphonic acids for efficient water permeation.

A series of organic phosphonic acids (OPAs) were applied as multifunctional spacers to enlarge the inner space of carbide MXene (Ti3C2Tx) laminates. A synergistic improvement in permeance, rejection and stability is achieved via introducing OPA to create pillared laminates. This strategy provides a universal way to regulate transport channels of MXene-based membranes.