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

Controllablesynthesis of nanoscale high-entropy alloys (HEAs)with specific morphologies and tunable compositions is crucial forexploring advanced catalysts. The present strategies either have greatdifficulties to tailor the morphology of nanoscale HEAs or sufferfrom narrow elemental distributions and insufficient generality. Toovercome the limitations of these strategies, here we report a robusttemplate-directed synthesis to programmatically fabricate nanoscaleHEAs with controllable compositions and structures via independentlycontrolling 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), 3Dnanodendrites, and vast elemental compositions combining five or moreof 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-artelectrocatalytic performance for the ethanol oxidation reaction, with25.6- and 16.3-fold improvements in mass activity, relative to commercialPd/C and Pt/C catalysts, respectively, as well as greatly enhanceddurability. This work provides a myriad of nanoscale HEAs and a generalsynthetic strategy, which are expected to have broad impacts for thefields of catalysis, sensing, biomedicine, and even beyond.

Automated summary

We report a template-directed synthesis method to programmatically fabricate nanoscale high-entropy alloys (HEAs) with controllable compositions and structures by independently controlling the morphology and composition of HEA. A total of 12 nanoscale HEAs with controllable morphologies including zero-dimension nanoparticles, one-dimensional nanowires, two-dimensional ultrathin nanorings (UNRs), and three-dimensional nanodendrites were synthesized. The as-prepared HEA-PdPtCuPbBiUNRs/C showed superior electrocatalytic performance for ethanol oxidation reaction, outperforming commercial Pd/C and Pt/C catalysts in terms of mass activity and durability. This work provides a wide range of nanoscale HEAs and a versatile synthetic strategy with potential impacts in catalysis, sensing, biomedicine, and beyond.