Programmable Synthesis of High-Entropy Nanoalloys for Efficient Ethanol Oxidation Reaction

ACS Nano. 2023 Jul 25;17(14):13659-13671. doi: 10.1021/acsnano.3c02762. Epub 2023 Jul 7.

Abstract

Controllable synthesis of nanoscale high-entropy alloys (HEAs) with specific morphologies and tunable compositions is crucial for exploring advanced catalysts. The present strategies either have great difficulties to tailor the morphology of nanoscale HEAs or suffer from narrow elemental distributions and insufficient generality. To overcome the limitations of these strategies, here we report a robust template-directed synthesis to programmatically fabricate nanoscale HEAs with controllable compositions and structures via independently controlling the morphology and composition of HEA. As a proof of concept, 12 kinds of nanoscale HEAs with controllable morphologies of zero-dimension (0D) nanoparticles, 1D nanowires, 2D ultrathin nanorings (UNRs), 3D nanodendrites, and vast elemental compositions combining five or more of Pd/Pt/Ag/Cu/Fe/Co/Ni/Pb/Bi/Sn/Sb/Ge are synthesized. Moreover, the as-prepared HEA-PdPtCuPbBiUNRs/C demonstrates the state-of-the-art electrocatalytic performance for the ethanol oxidation reaction, with 25.6- and 16.3-fold improvements in mass activity, relative to commercial Pd/C and Pt/C catalysts, respectively, as well as greatly enhanced durability. This work provides a myriad of nanoscale HEAs and a general synthetic strategy, which are expected to have broad impacts for the fields of catalysis, sensing, biomedicine, and even beyond.

Keywords: controllable compositions and structures; electrocatalysis; ethanol oxidation reaction; high-entropy nanoalloys; programmable synthesis; template-directed synthesis.