Origin of Chemically Ordered Atomic Laminates ( i-MAX): Expanding the Elemental Space by a Theoretical/Experimental Approach.

Dahlqvist, Martin; Petruhins, Andrejs; Lu, Jun; Hultman, Lars; Rosen, Johanna · ACS Nano · 2018

basic_science · Level V

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Abstract

With increased chemical diversity and structural complexity comes the opportunities for innovative materials possessing advantageous properties. Herein, we combine predictive first-principles calculations with experimental synthesis, to explore the origin of formation of the atomically laminated i-MAX phases. By probing (Mo<sub>2/3</sub> M<sub>1/3</sub><sup>2</sup>)<sub>2</sub> AC (where M<sup>2</sup> = Sc, Y and A = Al, Ga, In, Si, Ge, In), we predict seven stable i-MAX phases, five of which should have a retained stability at high temperatures. (Mo<sub>2/3</sub>Sc<sub>1/3</sub>)<sub>2</sub>GaC and (Mo<sub>2/3</sub>Y<sub>1/3</sub>)<sub>2</sub>GaC were experimentally verified, displaying the characteristic in-plane chemical order of Mo and Sc/Y and Kagomé-like ordering of the A-element. We suggest that the formation of i-MAX phases requires a significantly different size of the two metals, and a preferable smaller size of the A-element. Furthermore, the population of antibonding orbitals should be minimized, which for the metals herein (Mo and Sc/Y) means that A-elements from Group 13 (Al, Ga, In) are favored over Group 14 (Si, Ge, Sn). Using these guidelines, we foresee a widening of elemental space for the family of i-MAX phases and expect more phases to be synthesized, which will realize useful properties. Furthermore, based on i-MAX phases as parent materials for 2D MXenes, we also expect that the range of MXene compositions will be expanded.