Theoretical Analysis, Synthesis, and Characterization of 2D W_1.33C (MXene) with Ordered Vacancies

Abstract

Synthesis of delaminated 2D W1.33C (MXene) has been performed by selectively etching Al as well as Sc/Y from the recently discovered nanolaminated i-MAX phases (W2/3Sc1/3)2AlC and (W2/3Y1/3)2AlC. Both quaternary phases produce MXenes with similar flake morphology and with a skeletal structure due to formation of ordered vacancies. The measured O, OH, and F terminations, however, differ in amount as well as in relative ratios, depending on parent material, evident from X-ray photoelectron spectroscopy. These findings are correlated to theoretical simulations based on first-principles, investigating the W1.33C, and the effect of termination configurations on structure, formation energy, stability, and electronic structure. The theoretical results indicate a favored F-rich surface composition, though with a system going from insulating/semiconducting to metallic for different termination configurations, suggesting a high tuning potential of these materials. Additionally, free-standing W1.33C films of 2–4 μm thickness and with up to 10 wt % polymer (PEDOT:PSS) were tested as electrodes in supercapacitors, showing capacitances up to 600 F cm–3 in 1 M H2SO4 and high capacitance retention for at least 10000 cycles at 10 A g–1. This is highly promising results compared to other W-based materials to date.