Abstract
Research on low-dimensional materials has increased drastically in the last decade, with the discovery of two-dimensional transition metal carbides and nitrides (MXenes) produced by atom-selective chemical etching of laminated parent Mn+1AXn (MAX) phases. Here, we apply density functional theory and subsequent materials synthesis and analysis to explore the phase stability and Mo/Sc intermixing on the M site in the chemically ordered quaternary i−MAX phase (MoxSc1−x)2AlC. Transmission electron microscopy confirms the theoretical predictions of preferential in-plane ordering of Mo and Sc, with the highest crystal quality obtained for the ideal Mo:Sc ratio of 2:1 (predicted as the most stable), as well as a retained i−MAX structure even for an increased relative Sc content, with Sc partially occupying Mo sites. The results are supported by refined neutron diffraction data, which show space group C2/c (no. 15), and a C occupancy of 1. Subsequent chemical etching produces MXene for x=0.66, while for x=0.33 and 0.5 no MXene is observed. These results demonstrate that a precise control of the i−MAX composition is crucial for derivation of MXene, with a MXene quality optimized for a Mo:Sc ratio of 2:1 with minimal intermixing between Mo and Sc.
