Pre-Sodiated Ti₃C₂T_x MXene Structure and Behavior as Electrode for Sodium-Ion Capacitors

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Abstract

Layered titanium carbide (Ti₃C₂T_x) MXene is a promising electrode material for use in next-generation electrochemical capacitors. However, the atomic-level information needed to correlate the distribution of intercalated cations with surface redox reactions, has not been investigated in detail. Herein we report on sodium preintercalated MXene with high sodium content (up to 2Na per Ti₃C₂T_x formula) using a solution of Na-biphenyl radical anion complex (E0 ≈ -2.6 SHE). Multiple sodiation sites and formation of a two-dimensional sodium domain structure at interfaces/surfaces is identified through combined computational simulations with neutron pair distribution function analysis. The induced layer charges and the redox process characterized by the density-functional tight-binding method on a local scale are found to greatly depend on the location of sodium ions. Electrochemical testing of the pre-sodiated MXene as an electrode material in a sodium-ion capacitor shows excellent reversibility and promising performance, indicating the feasibility of chemical preintercalation as an approach to prepare MXene electrodes for ion capacitors.

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