Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts

Abstract

High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on the origin of their outstanding performance and the accurate identification of active centers. Herein, we report a conceptual and experimental approach to overcome the limitations of single-element catalysts by designing a FeCoNiXRu (X: Cu, Cr, and Mn) High-entropy alloys system with various active sites that have different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements in HEA induce significant charge redistribution and create highly active Co and Ru sites with optimized energy barriers for simultaneously stabilizing OH* and H* intermediates, which greatly enhances the efficiency of water dissociation in alkaline conditions. This work provides an in-depth understanding of the interactions between specific active sites and intermediates, which opens up a fascinating direction for breaking scaling relation issues for multistep reactions.

A Mean‐Field Model for Oxygen Reduction Electrocatalytic Activity on High‐Entropy Alloys**

“…Some attempts to obtain trends within fixed-element composition spaces have been investigated both experimentally [8][9][10][11] and theoretically. [5,[12][13][14] While some studies have attempted to discover trends in the constituent elements for a given catalyzed reaction, [15][16][17] finding appropriate descriptors for which elements to mix for optimal catalysis remains a challenge.…”

Facile synthesis of a novel 0D/2D CdS/Bi4TaO8Br heterojunction for enhanced photocatalytic tetracycline hydrochloride degradation under visible light

“…The bandgap structures of pure CdS, pure Bi 4 TaO 8 Br, and CdS/Bi 4 TaO 8 Br-200 were identified by Mott-Schottky curves. 48 As shown in were À0.83 eV, À0.6 eV, and À0.69 eV, respectively, which can be regarded as the conduction band position because the FB potential is on the verge of the conduction band (CB) for n-type semiconductors. 28 The CB position of the CdS/Bi 4 TaO 8 Br composite is between CdS and Bi 4 TaO 8 Br, which also indicates the formation of a heterojunction structure.…”

Atomic‐Level Design of Active Site on Two‐Dimensional MoS2 toward Efficient Hydrogen Evolution: Experiment, Theory, and Artificial Intelligence Modelling

“…Due to the insufficient comprehension in revealing practical atomistic structure and catalytic mechanisms of active sites from multiple dimensions, the structure-activity relationships of nanocatalysts still lack understanding. [6,7] At present, the concept of atomic structure and mechanism-oriented catalyst design in industrial-scale have gradually penetrated into the research community. [8] Thus, a comprehensive understanding of structure-activity relationships is of tremendous significance for the rational design of catalysts with specific active-site structure and function, the regulation of surface and interface reaction process, and the modulation of the selectivity and stability of catalysts.…”