Synthesis, properties and catalytic performance of the novel, pseudo-spinel, multicomponent transition-metal selenides

Abstract

With electrocatalysis being the very foundation of multiple energy conversion technologies, the search for more effective, and affordable catalysts is becoming increasingly important for their further development. Recently, the multicomponent approach, together with the electronic structure calculations, have established themselves as promising ways of designing such materials. In the presented study, both these approaches are combined, leading to the development of a unprecedented (Co,Fe,Ni)₃Se₄ chalcogenide catalyst. Based on the extensive density functional theory calculations (DFT), and structural data, the impact of the multi-element atomic arrangement is discussed, and the possible benefits of such a design strategy are identified. The transport and catalytic properties of the materials are studied, showing excellent charge transfer capabilities, combined with very high catalytic activity with regard to the hydrogen evolution reaction (HER), as evidenced by the current densities of 120, 500, and 1000 mA cm⁻² at overpotentials of 250, 360, and 450 mV. Of importance, all these results are achieved for the bulk-type electrode, obtained by a simple and scalable process, a considerable advantage over most of the state-of-the-art electrocatalysts, requiring costly and time-consuming nano-structuring of the electrode layer.